Graphene Oxide‐Templated Conductive and Redox‐Active Nanosheets Incorporated Hydrogels for Adhesive Bioelectronics

2D conductive nanosheets are central to electronic applications because of their large surface areas and excellent electronic properties. However, tuning the multifunctions and hydrophilicity of conductive nanosheets are still challenging. Herein, a green strategy is developed for fabricating conductive, redox‐active, water‐soluble nanosheets via the self‐assembly of poly(3,4‐ethylenedioxythiophene) (PEDOT) on the polydopamine‐reduced and sulfonated graphene oxide (PSGO) template. The conductivity and hydrophilicity of nanosheets are highly improved by PSGO. The nanosheets are redox active due to the abundant catechol groups and can be used as versatile nanofillers in developing conductive and adhesive hydrogels. The nanosheets create a mussel‐inspired redox environment inside the hydrogel networks and endow the hydrogel with long‐term and repeatable adhesiveness. This hydrogel is biocompatible and can be implanted for biosignals detection in vivo. This mussel‐inspired strategy for assembling 2D nanosheets can be adapted for producing diverse multifunctional nanomaterials, with various potential applications in bioelectronics.     

Mussel‐Inspired Adhesive and Conductive Hydrogel with Long‐Lasting Moisture and Extreme Temperature Tolerance

Conductive hydrogels are a promising class of materials to design bioelectronics for new technological interfaces with human body, which are required to work for a long‐term or under extreme environment. Traditional hydrogels are limited in short‐term usage under room temperature, as it is difficult to retain water under cold or hot environment. Inspired by the antifreezing/antiheating behaviors from nature, and based on mussel chemistry, an adhesive and conductive hydrogel is developed with long‐lasting moisture lock‐in capability and extreme temperature tolerance, which is formed in a binary‐solvent system composed of water and glycerol. Polydopamine (PDA)‐decorated carbon nanotubes (CNTs) are incorporated into the hydrogel, which assign conductivity to the hydrogel and serve as nanoreinforcements to enhance the mechanical properties of the hydrogel. The catechol groups on PDA and viscous glycerol endow the hydrogel with high tissue adhesiveness. Particularly, the hydrogel is thermal tolerant to maintain all the properties under extreme wide tempreature spectrum (?20 or 60 °C) or stored for a long term. In summary, this mussel‐inspired hydrogel is a promising material for self‐adhesive bioelectronics to detect biosignals in cold or hot environments, and also as a dressing to protect skin from injuries related to frostbites or burns.     

Ascidian‐Inspired Fast‐Forming Hydrogel System for Versatile Biomedical Applications: Pyrogallol Chemistry for Dual Modes of Crosslinking Mechanism

Exploitation of unique biochemical and biophysical properties of marine organisms has led to the development of functional biomaterials for various biomedical applications. Recently, ascidians have received great attention, owing to their extraordinary properties such as strong underwater adhesion and rapid self‐regeneration. Specific polypeptides containing 3,4,5‐trihydroxyphenylalanine (TOPA) in the blood cells of ascidians are associated with such intrinsic properties generated through complex oxidative processes. In this study, a bioinspired hydrogel platform is developed, demonstrating versatile applicability for tissue engineering and drug delivery, by conjugating pyrogallol (PG) moiety resembling ascidian TOPA to hyaluronic acid (HA). The HA–PG conjugate can be rapidly crosslinked by dual modes of oxidative mechanisms using an oxidant or pH control, resulting in hydrogels with different mechanical and physical characteristics. The versatile utility of HA–PG hydrogels formed via different crosslinking mechanisms is tested for different biomedical platforms, including microparticles for sustained drug delivery and tissue adhesive for noninvasive cell transplantation. With extraordinarily fast and different routes of PG oxidation, ascidian‐inspired HA–PG hydrogel system may provide a promising biomaterial platform for a wide range of biomedical applications.     

A Biomimetic Mussel‐Inspired ε‐Poly‐l‐lysine Hydrogel with Robust Tissue‐Anchor and Anti‐Infection Capacity

In situ hydrogels have attracted considerable attention in tissue engineering because of their minimal invasiveness and ability to match the irregular tissue defects. However, hydrous physiological environments and the high level of moisture in hydrogels severely hamper binding to the target tissue and easily cause wound infection, thereby limiting the effectiveness in wound care management. Thus, forming an intimate assembly of the hydrogel to the tissue and preventing wound infecting still remains a significant challenge. In this study, inspired by mussel adhesive protein, a biomimetic dopamine‐modified ε‐poly‐l ‐lysine‐polyethylene glycol‐based hydrogel (PPD hydrogel) wound dressing is developed in situ using horseradish peroxidase cross‐linking. The biomimetic catechol–Lys residue distribution in PPD polymer provides a catechol–Lys cooperation effect, which endows the PPD hydrogels with superior wet tissue adhesion properties. It is demonstrated that the PPD hydrogel can facilely and intimately integrate with biological tissue and exhibits superior capacity of in vivo hemostatic and accelerated wound repair. In addition, the hydrogels exhibit outstanding anti‐infection property because of the inherent antibacterial ability of ε‐poly‐l ‐lysine. These findings shed new light on the development of mussel‐inspired tissue‐anchored and antibacterial hydrogel materials serving as wound dressings.     

Bioinspired Double‐Dynamic‐Bond Crosslinked Bioadhesive Enables Post‐Wound Closure Care

Most existing bioadhesives, even those showing superiority in wound closure effectiveness, do not assist in the post‐wound closure process. A bioinspired, in situ formed, double‐dynamic‐bond crosslinked hydrogel bioadhesive that is capable of efficiently closing open wounds and enabling post‐wound closure care is reported. Catechol‐modified ε‐poly‐l ‐lysine and oxidized dextran are employed as natural polymer backbones and they are in situ crosslinked using Schiff's base dynamic bond and catechol? Fe coordinate dynamic bond through a process inspired by that used to cure marine mussel glue, forming a hydrogel bioadhesive. The unique double‐dynamic‐bond crosslinked structure endows the bioadhesive with higher mechanical and adhesive strength while retaining quick dissociation and good self‐healing capacities. Accordingly, the bioadhesive can exhibit multiple desirable functions, such as dissolution on demand, repeatable adhesiveness, adhesive and mechanical strength sufficient for wound closure, injectability, and good biocompatibility (DREAMING). After efficiently closing skin incisions, the bioadhesive can be facilely removed or repeatedly close the reopened wounds, thus enabling post‐wound closure care. On the basis of favorable functions in wound closure and the ability to enable post‐wound closure care, the bioadhesive demonstrates great potential in dealing with skin wounds.     

Wearable,Healable, and Adhesive Epidermal Sensors Assembled from Mussel‐Inspired Conductive Hybrid Hydrogel Framework

Healable, adhesive, wearable, and soft human‐motion sensors for ultrasensitive human–machine interaction and healthcare monitoring are successfully assembled from conductive and human‐friendly hybrid hydrogels with reliable self‐healing capability and robust self‐adhesiveness. The conductive, healable, and self‐adhesive hybrid network hydrogels are prepared from the delicate conformal coating of conductive functionalized single‐wall carbon nanotube (FSWCNT) networks by dynamic supramolecular cross‐linking among FSWCNT, biocompatible polyvinyl alcohol, and polydopamine. They exhibit fast self‐healing ability (within 2 s), high self‐healing efficiency (99%), and robust adhesiveness, and can be assembled as healable, adhesive, and soft human‐motion sensors with tunable conducting channels of pores for ions and framework for electrons for real time and accurate detection of both large‐scale and tiny human activities (including bending and relaxing of fingers, walking, chewing, and pulse). Furthermore, the soft human‐motion sensors can be enabled to wirelessly monitor the human activities by coupling to a wireless transmitter. Additionally, the in vitro cytotoxicity results suggest that the hydrogels show no cytotoxicity and can facilitate cell attachment and proliferation. Thus, the healable, adhesive, wearable, and soft human‐motion sensors have promising potential in various wearable, wireless, and soft electronics for human–machine interfaces, human activity monitoring, personal healthcare diagnosis, and therapy.     

Bio‐Inspired Stretchable,Adhesive, and Conductive Structural Color Film for Visually Flexible Electronics

The rapid progress in flexible electronic devices has attracted immense interest in many applications, such as health monitoring devices, sensory skins, and implantable apparatus. Here, inspired by the adhesion features of mussels and the color shift mechanism of chameleons, a novel stretchable, adhesive, and conductive structural color film is presented for visually flexible electronics. The film is generated by adding a conductive carbon nanotubes polydopamine (PDA) filler into an elastic polyurethane (PU) inverse opal scaffold. Owing to the brilliant flexibility and inverse opal structure of the PU layer, the film shows stable stretchability and brilliant structural color. Besides, the catechol groups on PDA impart the film with high tissue adhesiveness and self‐healing capability. Notably, because of its responsiveness, the resultant film is endowed with color‐changing ability that responds to motions, which can function as dual‐signal soft human‐motion sensors for real‐time color‐sensing and electrical signal monitoring. These features make the bio‐inspired hydrogel‐based electronics highly potential in the flexible electronics field.     

Self‐Hydrophobization in a Dynamic Hydrogel for Creating Nonspecific Repeatable Underwater Adhesion

Adhesive hydrogels are widely applied for biological and medical purposes; however, they are generally unable to adhere to tissues under wet/underwater conditions. Herein, described is a class of novel dynamic hydrogels that shows repeatable and long‐term stable underwater adhesion to various substrates including wet biological tissues. The hydrogels have Fe³⁺‐induced hydrophobic surfaces, which are dynamic and can undergo a self‐hydrophobization process to achieve strong underwater adhesion to a diverse range of dried/wet substrates without the need for additional processes or reagents. It is also demonstrated that the hydrogels can directly adhere to biological tissues in the presence of under sweat, blood, or body fluid exposure, and that the adhesion is compatible with in vivo dynamic movements. This study provides a novel strategy for fabricating underwater adhesive hydrogels for many applications, such as soft robots, wearable devices, tissue adhesives, and wound dressings.     

Skin‐Inspired Antibacterial Conductive Hydrogels for Epidermal Sensors and Diabetic Foot Wound Dressings

Recently, artificial intelligence research has driven the development of stretchable and flexible electronic systems. Conductive hydrogels are a class of soft electronic materials that have emerging applications in wearable and implantable biomedical devices. However, current conductive hydrogels possess fundamental limitations in terms of their antibacterial performance and a mechanical mismatch with human tissues, which severely limits their applications in biological interfaces. Here, inspired by animal skin, a conductive hydrogel is fabricated from a supramolecular assembly of polydopamine decorated silver nanoparticles (PDA@Ag NPs), polyaniline, and polyvinyl alcohol, namely PDA@Ag NPs/CPHs. The resultant hydrogel has many desirable features, such as tunable mechanical and electrochemical properties, eye‐catching processability, good self‐healing ability as well as repeatable adhesiveness. Remarkably, PDA@Ag NPs/CPHs exhibit broad antibacterial activity against Gram‐negative and Gram‐positive bacteria. The potential application of this versatile hydrogel is demonstrated by monitoring large‐scale movements of the human body in real time. In addition, PDA@Ag NPs/CPHs have a significant therapeutic effect on diabetic foot wounds by promoting angiogenesis, accelerating collagen deposition, inhibiting bacterial growth, and controlling wound infection. To the best of the authors' knowledge, this is the first time that conductive hydrogels with antibacterial ability are developed for use as epidermal sensors and diabetic foot wound dressing.     

Supramolecular β‐Sheet Suckerin–Based Underwater Adhesives

Nature has evolved several molecular strategies to ensure adhesion in aqueous environments, where artificial adhesives typically fail. One recently‐unveiled molecular design for wet‐resistant adhesion is the cohesive cross‐β structure characteristic of amyloids, complementing the well‐established surface‐binding strategy of mussel adhesive proteins based on 3,4‐l ‐dihydroxyphenylalanine (Dopa). Structural proteins that self‐assemble into cross β‐sheet networks are the suckerins discovered in the sucker ring teeth of squids. Here, light is shed on the wet adhesion of cross‐β motifs by producing recombinant suckerin‐12, naturally lacking Dopa, and investigating its wet adhesion properties. Surprisingly, the adhesion forces measured on mica reach 70 mN m^?1, exceeding those measured for all mussel adhesive proteins to date. The pressure‐sensitive adhesion of artificial suckerins is largely governed by their cross‐β motif, as evidenced using control experiments with disrupted cross‐β domains that result in complete loss of adhesion. Dopa is also incorporated in suckerin‐12 using a residue‐specific incorporation strategy that replaces tyrosine with Dopa during expression in Escherichia coli. Although the replacement does not increase the long‐term adhesion, it contributes to the initial rapid contact and enhances the adsorption onto model oxide substrates. The findings suggest that suckerins with supramolecular cross‐β motifs are promising biopolymers for wet‐resistant adhesion.     

Mussel Inspired Dynamic Cross‐Linking of Self‐Healing Peptide Nanofiber Network

A general drawback of supramolecular peptide networks is their weak mechanical properties. In order to overcome a similar challenge, mussels have adapted to a pH‐dependent iron complexation strategy for adhesion and curing. This strategy also provides successful stiffening and self‐healing properties. The present study is inspired by the mussel curing strategy to establish iron cross‐link points in self‐assembled peptide networks. The impact of peptide‐iron complexation on the morphology and secondary structure of the supramolecular nanofibers is characterized by scanning electron microscopy, circular dichroism and Fourier transform infrared spectroscopy. Mechanical properties of the cross‐linked network are probed by small angle oscillatory rheology and nanoindentation by atomic force microscopy. It is shown that iron complexation has no influence on self‐assembly and β‐sheet‐driven elongation of the nanofibers. On the other hand, the organic‐inorganic hybrid network of iron cross‐linked nanofibers demonstrates strong mechanical properties comparable to that of covalently cross‐linked network. Strikingly, iron cross‐linking does not inhibit intrinsic reversibility of supramolecular peptide polymers into disassembled building blocks and the self‐healing ability upon high shear load. The strategy described here could be extended to improve mechanical properties of a wide range of supramolecular polymer networks.     

Tissue Adhesive Catechol‐Modified Hyaluronic Acid Hydrogel for Effective,Minimally Invasive Cell Therapy

Current hyaluronic acid (HA) hydrogel systems often cause cytotoxicity to encapsulated cells and lack the adhesive property required for effective localization of transplanted cells in vivo. In addition, the injection of hydrogel into certain organs (e.g., liver, heart) induces tissue damage and hemorrhage. In this study, we describe a bioinspired, tissue‐adhesive hydrogel that overcomes the limitations of current HA hydrogels through its improved biocompatibility and potential for minimally invasive cell transplantation. HA functionalized with an adhesive catecholamine motif of mussel foot protein forms HA‐catechol (HA‐CA) hydrogel via oxidative crosslinking. HA‐CA hydrogel increases viability, reduces apoptosis, and enhances the function of two types of cells (human adipose‐derived stem cells and hepatocytes) compared with a typical HA hydrogel crosslinked by photopolymerization. Due to the strong tissue adhesiveness of the HA‐CA hydrogel, cells are easily and efficiently transplanted onto various tissues (e.g., liver and heart) without the need for injection. Stem cell therapy using the HA‐CA hydrogel increases angiogenesis in vivo, leading to improved treatment of ischemic diseases. HA‐CA hydrogel also improved hepatic functions of transplanted hepatocytes in vivo. Thus, this bioinspired, tissue‐adhesive HA hydrogel can enhance the efficacy of minimally invasive cell therapy.     

Mussel‐Inspired Approach to Constructing Robust Multilayered Alginate Films for Antibacterial Applications

The exceptional mechanical properties of the byssus—the fibrous holdfast of mussels that provides underwater adhesion—have potential applications in medicine and technology. The catechol–Fe³⁺–catechol interaction underlies the unique properties of mussel byssus and has emerged as a tool for developing functional hybrid materials such as pH‐responsive, self‐healing gels. Herein, the construction of functional alginate (Alg) film on a solid substrate inspired by mussel byssus is reported. The approach consists of spin‐coating‐assisted deposition of Alg catechols onto a solid substrate and their subsequent crosslinking via catechol–Fe³⁺–catechol interactions. This yields robust and multilayered Alg films that are resistant to protein adsorption and suppress bacterial adhesion. This method can be used to create antibacterial films for coating implanted medical devices.     

Ultracompliant Hydrogel‐Based Neural Interfaces Fabricated by Aqueous‐Phase Microtransfer Printing

Hydrogel‐based electronics are ideally suited for neural interfaces because they exhibit ultracompliant mechanical properties that match that of excitable tissue in the brain and peripheral nerve. Hydrogel‐based multielectrode arrays (MEAs) can conformably interface with tissues to minimize inflammation and improve the reliability to enhance signal transduction. However, MEA substrates composed of swollen hydrogels exhibit low toughness and poor adhesion when laminated on the tissue surface and also present incompatibilities with processes commonly used in MEA fabrication. Here, a strategy to fabricate an ultracompliant MEA is described based on aqueous‐phase transfer printing. This technique employs redox active adhesive motifs in hygroscopic polymer precursors that simultaneously form hydrogels through sol–gel phase transitions and bond to materials in the underlying microelectronic structures. Specifically, in situ gelation of four‐arm‐polyethylene glycol‐grafted catechol [PEG‐Dopa]₄ hydrogels induced by oxidation using Fe³⁺ produces conformal adhesive contact with the underlying MEA, robust adhesion to electronic sub‐structures, and rapid dissolution of water‐soluble sacrificial release layers. MEAs are integrated on hydrogel‐based substrates to produce free‐standing ultracompliant neural probes, which are then laminated to the surface of the dorsal root ganglia in feline subjects to record single‐unit neural activity.     

Highly Efficient Self‐Healable and Dual Responsive Cellulose‐Based Hydrogels for Controlled Release and 3D Cell Culture

To face the increasing demand of self‐healing hydrogels with biocompatibility and high performances, a new class of cellulose‐based self‐healing hydrogels are constructed through dynamic covalent acylhydrazone linkages. The carboxyethyl cellulose‐graft‐dithiodipropionate dihydrazide and dibenzaldehyde‐terminated poly(ethylene glycol) are synthesized, and then the hydrogels are formed from their mixed solutions under 4‐amino‐DL‐phenylalanine (4a‐Phe) catalysis. The chemical structure, as well as microscopic morphologies, gelation times, mechanical and self‐healing performances of the hydrogels are investigated with ¹H NMR, Fourier transform infrared spectroscopy, atomic force microscopy, rheological and compression measurements. Their gelation times can be controlled by varying the total polymer concentration or 4a‐Phe content. The resulted hydrogels exhibit excellent self‐healing ability with a high healing efficiency (≈96%) and good mechanical properties. Moreover, the hydrogels display pH/redox dual responsive sol‐gel transition behaviors, and are applied successfully to the controlled release of doxorubicin. Importantly, benefitting from the excellent biocompatibility and the reversibly cross‐linked networks, the hydrogels can function as suitable 3D culture scaffolds for L929 cells, leading to the encapsulated cells maintaining a high viability and proliferative capacity. Therefore, the cellulose‐based self‐healing hydrogels show potential applications in drug delivery and 3D cell culture for tissue engineering.     

Hyaluronic Acid Catechol: A Biopolymer Exhibiting a pH‐Dependent Adhesive or Cohesive Property for Human Neural Stem Cell Engineering

Nature has developed materials that are integrated and effective at controlling their properties of adhesiveness and cohesiveness; the chemistry of these materials has been optimized during evolution. For example, a catechol moiety found in the adhesive proteins of marine mussels regulates its properties between adhesion and cohesion, rapidly adapting to environmental conditions. However, in synthetic materials chemistry, introduced chemical moieties are usually monofunctional, either being adhesive or cohesive; typically, this is not effective compared to natural materials. Herein, it is demonstrated that hyaluronic acid‐catechol (HA‐catechol) conjugates can exhibit either adhesiveness, functionalizing the surface of materials, or cohesiveness, building 3D hydrogels. Up to now, catechol‐conjugated polymers have shown to be useful in one of these two functions. The usefulness of the polymer in stem cell engineering is demonstrated. A platform for neural stem cell culture may be prepared, utilizing the adhesive property of HA‐catechol, and hydrogels are fabricated to encapsulate the neural stem cells, utilizing the cohesive property of the HA conjugate. Moreover, the HA‐catechol hydrogels are highly neural stem cell compatible, showing better viability compared to existing methods based on HA hydrogels.     

A Highly Elastic and Rapidly Crosslinkable Elastin‐Like Polypeptide‐Based Hydrogel for Biomedical Applications

Elastin‐like polypeptides (ELPs) are promising for biomedical applications due to their unique thermoresponsive and elastic properties. ELP‐based hydrogels have been produced through chemical and enzymatic crosslinking or photocrosslinking of modified ELPs. Herein, a photocrosslinked ELP gel using only canonical amino acids is presented. The inclusion of thiols from a pair of cysteine residues in the ELP sequence allows disulfide bond formation upon exposure to UV light, leading to the formation of a highly elastic hydrogel. The physical properties of the resulting hydrogel such as mechanical properties and swelling behavior can be easily tuned by controlling ELP concentrations. The biocompatibility of the engineered ELP hydrogels is shown in vitro as well as corroborated in vivo with subcutaneous implantation of hydrogels in rats. ELP constructs demonstrate long‐term structural stability in vivo, and early and progressive host integration with no immune response, suggesting their potential for supporting wound repair. Ultimately, functionalized ELPs demonstrate the ability to function as an in vivo hemostatic material over bleeding wounds.     

Conductive MXene Nanocomposite Organohydrogel for Flexible,Healable, Low‐Temperature Tolerant Strain Sensors

Conductive hydrogels are attracting tremendous interest in the field of flexible and wearable soft strain sensors because of their great potential in electronic skins, and personalized healthcare monitoring. However, conventional conductive hydrogels using pure water as the dispersion medium will inevitably freeze at subzero temperatures, resulting in the diminishment of their conductivity and mechanical properties; meanwhile, even at room temperature, such hydrogels suffer from the inevitable loss of water due to evaporation, which leads to a poor shelf‐life. Herein, an antifreezing, self‐healing, and conductive MXene nanocomposite organohydrogel (MNOH) is developed by immersing MXene nanocomposite hydrogel (MNH) in ethylene glycol (EG) solution to replace a portion of the water molecules. The MNH is prepared from the incorporation of the conductive MXene nanosheet networks into hydrogel polymer networks. The as‐prepared MNOH exhibits an outstanding antifreezing property (?40 °C), long‐lasting moisture retention (8 d), excellent self‐healing capability, and superior mechanical properties. Furthermore, this MNOH can be assembled as a wearable strain sensor to detect human biologic activities with a relatively broad strain range (up to 350% strain) and a high gauge factor of 44.85 under extremely low temperatures. This work paves the way for potential applications in electronic skins, human?machine interactions, and personalized healthcare monitoring.     

Bioinspired Adhesive Hydrogels Tackified by Nucleobases

Bioinspired strategies for designing hydrogels with excellent adhesive performance have drawn much attention in biomedical applications. Here, bioinspired adhesive hydrogels tackified by independent nucleobase (adenine, thymine, guanine, cytosine, and uracil) from DNA and RNA are successfully explored. The nucleobase‐tackified hydrogels exhibit an excellent adhesive behavior for not only various solid substrates (polytetrafluoroethylene, plastics, rubbers, glasses, metals, and woods) but also biological tissues consisting of heart, liver, spleen, lung, kidney, bone, and muscle. The maximum adhesion strength of A‐, T‐, G‐, C‐, and U‐tackified hydrogels on the aluminum alloy surface is 780, 166, 250, 227, and 433 N m^?1, respectively, superior to that of pure PAAm hydrogels (40 N m^?1) after adhesive time of 10 min. It is anticipated that bioinspired hydrogels will play a significant role in the applications of wound dressing, medical electrodes, tissue adhesives, and portable equipment. Moreover, the bioinspired nucleobase‐tackified strategy would open a novel avenue for designing the next generation of soft and adhesive materials.     

An Underwater Surface‐Drying Peptide Inspired by a Mussel Adhesive Protein

Water hampers the formation of strong and durable bonds between adhesive polymers and solid surfaces, in turn hindering the development of adhesives for biomedical and marine applications. Inspired by mussel adhesion, a mussel foot protein homologue (mfp3S‐pep) is designed, whose primary sequence is designed to mimic the pI, polyampholyte, and hydrophobic characteristics of the native protein. Noticeably, native protein and synthetic peptide exhibit similar abilities to self‐coacervate at given pH and ionic strength. 3,4‐dihydroxy‐l ‐phenylalanine (Dopa) proves necessary for irreversible peptide adsorption to both TiO₂ (anatase) and hydroxyapatite (HAP) surfaces, as confirmed by quartz crystal microbalance measurements, with the coacervate showing superior adsorption. The adsorption of Dopa‐containing peptides is investigated by attenuated total reflection infrared spectroscopy, revealing initially bidentate coordinative bonds on TiO₂, followed by H‐bonded and eventually long‐ranged electrostatic and Van der Waals interactions. On HAP, mfp3s‐pep‐3Dopa adsorption occurs predominantly via H‐bond and outersphere complexes of the catechol groups. Importantly, only the Dopa‐bearing compounds are able to remove interfacial water from the target surfaces, with the coacervate achieving the highest water displacement arising from its superior wetting properties. These findings provide an impetus for deve­loping coacervated Dopa‐functionalized peptides/polymers adhesive formulations for a variety of applications on wet polar surfaces.