Confinement of Thermoresponsive Hydrogels in Nanostructured Porous Silicon Dioxide Templates

A thermoresponsive hydrogel, poly(N‐isopropylacrylamide) (poly(NIPAM)), is synthesized in situ within an oxidized porous Si template, and the nanocomposite material is characterized. Infiltration of the hydrogel into the interconnecting nanoscale pores of the porous SiO₂ host is confirmed by scanning electron microscopy. The optical reflectivity spectrum of the nanocomposite hybrid displays Fabry–Pérot fringes characteristic of thin film interference, enabling direct, real‐time observation of the volume phase transition of the confined poly(NIPAM) hydrogel. Reversible optical reflectivity changes are observed to correlate with the temperature‐dependent volume phase transition of the hydrogel, providing a new means of studying nanoscale confinement of responsive hydrogels. The confined hydrogel displays a swelling and shrinking response to changes in temperature that is significantly faster than that of the bulk hydrogel. The porosity and pore size of the SiO₂ template, which are precisely controlled by the electrochemical synthesis parameters, strongly influence the extent and rate of changes in the reflectivity spectrum of the nanocomposite. The observed optical response is ascribed to changes in both the mechanical and the dielectric properties of the nanocomposite.     

Chitosan Hydrogel‐Capped Porous SiO2 as a pH Responsive Nano‐Valve for Triggered Release of Insulin

A pH responsive, chitosan‐based hydrogel film is used to cap the pores of a porous SiO₂ layer. The porous SiO₂ layer is prepared by thermal oxidation of an electrochemically etched Si wafer, and the hydrogel film is prepared by reaction of chitosan with glycidoxypropyltrimethoxysilane (GPTMS). Optical reflectivity spectroscopy and scanning electron microscopy (SEM) confirm that the bio‐polymer only partially infiltrates the porous SiO₂ film, generating a double layer structure. The optical reflectivity spectrum displays Fabry–Pérot interference fringes characteristic of a double layer, which is characterized using reflective interferometric Fourier transform spectroscopy (RIFTS). Monitoring the position of the RIFTS peak corresponding to the hydrogel layer allows direct, real‐time observation of the reversible volume phase transition of the hydrogel upon cycling of pH in the range 6.0–7.4. The swelling ratio and response time are controlled by the relative amount of GPTMS in the hydrogel. The pH‐dependent volume phase transition can be used to release insulin trapped in the porous SiO₂ layer underneath the hydrogel film. At pH 7.4, the gel in the top layer effectively blocks insulin release, while at pH 6.0 insulin penetrates the swollen hydrogel layer, resulting in a steady release into solution.     

Color Tunable Poly (N‐Isopropylacrylamide)‐co‐Acrylic Acid Microgel–Au Hybrid Assemblies

A new class of materials that are capable of color tunability over 300 nm with a 15 °C temperature change is introduced. The materials are assembled from thermoresponsive poly (N‐isopropylacrylamide)‐co‐acrylic acid (pNIPAm‐co‐AAc) microgels, which are deposited on Au coated glass substrates. The films are also pH responsive; the temperature‐induced color change was suppressed at high pH and is consistent with the behavior of a solution of suspended microgels. The mechanism proposed to account for the observed optical properties suggests that they result from the two Au layers being separated from each other by the “monolithic” microgel film, much like a Fabry‐Pérot etalon or interferometer. It is the modulation of the distance between these two layers, facilitated by the microgel collapse transition at high temperature, that allows the color to be tuned. The sensitivity of the system presented here will be used for future sensing and biosensing applications, as well as for light filtering applications.     

Programmed Deformations of 3D‐Printed Tough Physical Hydrogels with High Response Speed and Large Output Force

Shape‐morphing hydrogels have emerging applications in biomedical devices, soft robotics, and so on. However, successful applications require a combination of excellent mechanical properties and fast responding speed, which are usually a trade‐off in hydrogel‐based devices. Here, a facile approach to fabricate 3D gel constructs by extrusion‐based printing of tough physical hydrogels, which show programmable deformations with high response speed and large output force, is described. Highly viscoelastic poly(acrylic acid‐co‐acrylamide) (P(AAc‐co‐AAm)) and poly(acrylic acid‐co‐N‐isopropyl acrylamide) (P(AAc‐co‐NIPAm)) solutions or their mixtures are printed into 3D constructs by using multiple nozzles, which are then transferred into FeCl₃ solution to gel the structures by forming robust carboxyl–Fe³⁺ coordination complexes. The printed gel fibers containing poly(N‐isopropyl acrylamide) segment exhibit considerable volume contraction in concentrated saline solution, whereas the P(AAc‐co‐AAm) ones do not contract. The mismatch in responsiveness of the gel fibers affords the integrated 3D gel constructs the shape‐morphing ability. Because of the small diameter of gel fibers, the printed gel structures deform and recover with a fast speed. A four‐armed gripper is designed to clamp plastic balls with considerable holding force, as large as 115 times the weight of the gripper. This strategy should be applicable to other tough hydrogels and broaden their applications.     

Multivalent‐Ion‐Mediated Stabilization of Hydrogen‐Bonded Multilayers

Hydrogen‐bonding interactions are an important alternative to electrostatic interactions for assembling multilayer thin films of uncharged components. Herein, a new method is reported for rendering such films stable at pH values close to physiological conditions. Multilayer films based on hydrogen bonding are assembled by the alternate deposition of poly[(styrene sulfonic acid)‐co‐(maleic acid)] (PSSMA) and poly(N‐isopropylacrylamide) (PNiPAAm) at pH 2.5. The use of PSSMA results in multilayers that contain free styrene sulfonate groups, as these moieties do not interact with the PNiPAAm functional groups. Subsequent infiltration of a multivalent ion (Ce⁴⁺ or Fe³⁺) leads to an increase in the total film mass, with little impact on the film morphology, as determined by using atomic force microscopy. To examine the film stability, the resulting films have been exposed to elevated pH (7.1). While there is substantial swelling of the multilayers (25 % and 55 % for Ce⁴⁺‐ and Fe³⁺‐stabilized films, respectively), film loss is negligible. This provides a stark contrast with non‐stabilized films, which disassemble almost immediately upon exposure to pH 7.1. This method represents a simple and effective strategy for stabilizing hydrogen‐bonded structures non‐covalently. Further, the multivalent ions also render the films responsive to changes in the local redox environment, as demonstrated by film disassembly after exposure of Fe³⁺‐treated films to iodide solutions.     

Construction and Characterization of Porous SiO2/Hydrogel Hybrids as Optical Biosensors for Rapid Detection of Bacteria

The use of a new class of hybrid nanomaterials as label‐free optical biosensors for bacteria detection (E. coli K12 as a model system) is demonstrated. The hybrids combine a porous SiO₂ (PSiO₂) optical nanostructure (a Fabry–Pérot thin film) used as the optical transducer element and a hydrogel. The hydrogel, polyacrylamide, is synthesized in situ within the nanostructure inorganic host and conjugated with specific monoclonal antibodies (IgGs) to provide the active component of the biosensor. The immobilization of the IgGs onto the hydrogel via a biotin‐streptavidin system is confirmed by fluorescent labeling experiments and reflective interferometric Fourier transform spectroscopy (RIFTS). Additionally, the immobilized IgGs maintain their immunoactivity and specificity when attached to the sensor surface. Exposure of these modified‐hybrids to the target bacteria results in “direct cell capture” onto the biosensor surface. These specific binding events induce predictable changes in the thin‐film optical interference spectrum of the hybrid. Preliminary studies demonstrate the applicability of these biosensors for the detection of low bacterial concentrations in the range of 10³–10⁵ cell mL^?1 within minutes.     

Positively Thermo‐Sensitive Monodisperse Core–Shell Microspheres

In this paper, we report on a novel family of monodisperse thermo‐sensitive core–shell hydrogel microspheres that is featured with high monodispersity and positively thermo‐responsive volume phase transition characteristics with tunable swelling kinetics, i.e., the particle swelling is induced by an increase rather than a decrease in temperature. The microspheres were fabricated in a three‐step process. In the first step, monodisperse poly(acrylamide‐co‐styrene) seeds were prepared by emulsifier‐free emulsion polymerization. In the second step, poly(acrylamide) or poly[acrylamide‐co‐(butyl methacrylate)] shells were fabricated on the microsphere seeds by free radical polymerization. In the third step, the core–shell microspheres with poly‐ (acrylamide)/poly(acrylic acid) based interpenetrating polymer network (IPN) shells were finished by a method of sequential IPN synthesis. The proposed monodisperse core–shell microspheres provide a new mode of the phase transition behavior for thermo‐sensitive “smart” or “intelligent” monodisperse micro‐actuators that is highly attractive for targeting drug delivery systems, chemical separations, sensors, and so on.     

Organic Light‐Emitting Diodes Based on Poly(9,9‐dioctylfluorene‐co‐bithiophene) (F8T2)

A study of the optical properties of poly(9,9‐dioctylfluorene‐co‐bithiophene) (F8T2) is reported, identifying this polymer as one that possesses a desirable combination of charge transport and light emission properties. The optical and morphological properties of a series of polymer blends with F8T2 dispersed in poly(9,9‐dioctylfluorene) (PFO) are described and almost pure‐green emission from light emitting diodes (LEDs) based thereon is demonstrated. High luminance green electroluminescence from LEDs using only a thin film of F8T2 for emission is also reported. The latter demonstration for a polymer previously primarily of interest for effective charge transport constitutes an important step in the development of emissive materials for applications where a union of efficient light emission and effective charge transport is required.     

Positively K+‐Responsive Membranes with Functional Gates Driven by Host–Guest Molecular Recognition

A novel positively K⁺‐responsive membrane with functional gates driven by host‐guest molecular recognition is prepared by grafting poly(N‐isopropylacrylamide‐co‐acryloylamidobenzo‐15‐crown‐5) (poly(NIPAM‐co‐AAB₁₅C₅)) copolymer chains in the pores of porous nylon‐6 membranes with a two‐step method combining plasma‐induced pore‐filling grafting polymerization and chemical modification. Due to the cooperative interaction of host‐guest complexation and phase transition of the poly(NIPAM‐co‐AAB₁₅C₅), the grafted gates in the membrane pores could spontaneously switch from “closed” state to “open” state by recognizing K⁺ ions in the environment and vice versa; while other ions (e.g., Na⁺, Ca²⁺ or Mg²⁺) can not trigger such an ion‐responsive switching function. The positively K⁺‐responsive gating action of the membrane is rapid, reversible, and reproducible. The proposed K⁺‐responsive gating membrane provide a new mode of behavior for ion‐recognizable “smart” or “intelligent” membrane actuators, which is highly attractive for controlled release, chemical/biomedical separations, tissue engineering, sensors, etc.     

Multifunctional Up‐Converting Nanocomposites with Smart Polymer Brushes Gated Mesopores for Cell Imaging and Thermo/pH Dual‐Responsive Drug Controlled Release

Multifunctional nanocarriers based on the up‐conversion luminescent nanoparticles of NaYF₄:Yb³⁺/Er³⁺ core (UCNPs) and thermo/pH‐coupling sensitive polymer poly[(N‐isopropylacrylamide)‐co‐(methacrylic acid)] (P(NIPAm‐co‐MAA)) gated mesoporous silica shell are reported for cancer theranostics, including fluorescence imaging, and for controlled drug release for therapy. The as‐synthesized hybrid nanospheres UCNPs@mSiO₂‐P(NIPAm‐co‐MAA) show bright green up‐conversion fluorescence under 980 nm laser excitation and the thermo/pH‐sensitive polymer is active as a “valve” to moderate the diffusion of the embedded drugs in‐and‐out of the pore channels of the silica container. The anticancer drug doxorubicin hydrochloride (DOX) can be absorbed into UCNPs@mSiO₂‐P(NIPAm‐co‐MAA) nanospheres and the composite drug delivery system (DDS) shows a low level of leakage at low temperature/high pH values but significantly enhanced release at higher temperature/lower pH values, exhibiting an apparent thermo/pH controlled “on‐off” drug release pattern. The as‐prepared UCNPs@mSiO₂‐P(NIPAm‐co‐MAA) hybrid nanospheres can be used as bioimaging agents and biomonitors to track the extent of drug release. The reported multifunctional nanocarriers represent a novel and versatile class of platform for simultaneous imaging and stimuli‐responsive controlled drug delivery.     

Spray‐Coating Magnetic Thin Hybrid Films of PS‐b‐PNIPAM and Magnetite Nanoparticles

Spray coating is employed to fabricate magnetic thin films composed of the diblock copolymer polystyrene‐block‐poly(N‐isopropylacrylamide) and Fe₃O₄ magnetic nanoparticles (MNPs) functionalized with hydrophobic coatings. The kinetics of structure formation of the hybrid films is followed in situ with grazing incidence small angle X‐ray scattering during the spray deposition. To gain a better understanding of the influence of MNPs on the overall structure formation, the pure polymer film is also deposited as a reference via an identical spray protocol. At the initial spraying stage, the hybrid film (containing 2 wt% of MNPs) exhibits a faster formation process of a complete film as compared to the reference. The existence of MNPs depresses the dewetting behavior of polymer films on the substrate at macroscale and simultaneously alters the polymer microphase separation structure orientation from parallel to vertical. As spraying proceeds, MNPs aggregate into agglomerates with increasing sizes. After the spray deposition is finished, both samples gradually reach an equilibrium state and magnetic films with stable structures are achieved in the end. Superconducting quantum interference device investigation reveals the superparamagnetic property of the sprayed hybrid film. Consequently, potential application of sprayed films in fields such as magnetic sensors or data storage appears highly promising.     

Physical Double‐Network Hydrogel Adhesives with Rapid Shape Adaptability,Fast Self‐Healing,Antioxidant and NIR/pH Stimulus‐Responsiveness for Multidrug‐Resistant Bacterial Infection and Removable Wound Dressing

Developing physical double‐network (DN) removable hydrogel adhesives with both high healing efficiency and photothermal antibacterial activities to cope with multidrug‐resistant bacterial infection, wound closure, and wound healing remains an ongoing challenge. An injectable physical DN self‐healing hydrogel adhesive under physiological conditions is designed to treat multidrug‐resistant bacteria infection and full‐thickness skin incision/defect repair. The hydrogel adhesive consists of catechol–Fe³⁺ coordination cross‐linked poly(glycerol sebacate)‐co‐poly(ethylene glycol)‐g‐catechol and quadruple hydrogen bonding cross‐linked ureido‐pyrimidinone modified gelatin. It possesses excellent anti‐oxidation, NIR/pH responsiveness, and shape adaptation. Additionally, the hydrogel presents rapid self‐healing, good tissue adhesion, degradability, photothermal antibacterial activity, and NIR irradiation and/or acidic solution washing‐assisted removability. In vivo experiments prove that the hydrogels have good hemostasis of skin trauma and high killing ratio for methicillin‐resistant staphylococcus aureus (MRSA) and achieve better wound closure and healing of skin incision than medical glue and surgical suture. In particular, they can significantly promote full‐thickness skin defect wound healing by regulating inflammation, accelerating collagen deposition, promoting granulation tissue formation, and vascularization. These on‐demand dissolvable and antioxidant physical double‐network hydrogel adhesives are excellent multifunctional dressings for treating in vivo MRSA infection, wound closure, and wound healing.     

Polymer Thin‐Film Transistor Arrays Patterned by Stamping

We present a process to stamp semiconductor polymers suitable for the parallel fabrication of thin‐film transistor island arrays. This process is compatible with roll‐to‐roll fabrication. When a chemically treated elastomeric stamp is pressed against a substrate previously coated with the polymer solution, a capillary force drives the polymer solution into the stamp recesses. Simultaneously, the raised features of the stamp in contact with the substrate absorb the solvent. The resulting polymer thin film reproduces the pattern of the raised features of the stamp. Features with lateral dimensions as small as 2 μm are faithfully reproduced. We use this stamping process to fabricate arrays of polymer thin‐film transistors (TFTs) using poly(fluorene‐co‐bithiophene) and poly(thiophene) semiconductors.     

Generation of Compositional‐Gradient Structures in Biodegradable,Immiscible, Polymer Blends by Intermolecular Hydrogen‐Bonding Interactions

A biodegradable, immiscible poly(butylenes adipate‐co‐butylenes terephthalate) [P(BA‐co‐BT)]/poly(ethylene oxide) (PEO) polymer blend film with compositional gradient in the film‐thickness direction has been successfully prepared in the presence of a low‐molecular‐weight compound 4,4′‐thiodiphenal (TDP), which is used as a miscibility‐enhancing agent. The miscibilities of the P(BA‐co‐BT)/PEO/TDP ternary blend films and the P(BA‐co‐BT)/PEO/TDP gradient film were investigated by differential scanning calorimetry (DSC). The compositional gradient structure of the P(BA‐co‐BT)/PEO/TDP (46/46/8 w/w/w) film has been confirmed by microscopic mapping measurement of Fourier‐transform infrared spectra and dynamic mechanical thermal analysis. We have developed a new strategy for generating gradient‐phase structures in immiscible polymer‐blend systems by homogenization, i.e., adding a third agent that can enhance the miscibility of the two immiscible polymers through simultaneous formation of hydrogen bonds with two component polymers.     

Photocurrent enhancement in thin‐film silicon solar cells by combination of anti‐reflective sub‐wavelength structures and light‐trapping textures

Dielectric films with anti‐reflective sub‐wavelength structures are applied to thin‐film silicon solar cells to improve the light incoupling at the front surface. It is verified that modification of the refractive index of the incident medium using dielectric films with sub‐wavelength structures is beneficial to reduce the average reflectivity of Si solar cells with an anti‐reflective coating based on optical interference. It is also shown that the sub‐wavelength structure must be combined with a proper light‐trapping texture to enhance the absorption within thin‐film silicon solar cells. The effectiveness of dielectric films with sub‐wavelength structures is demonstrated by an increase of the short‐circuit current density of a microcrystalline silicon cell from 29.1 to 30.4 mA/cm² in a designated area of 1 cm². The optical interplay between the dielectric films and the light‐trapping textures is also discussed. Copyright © 2015 John Wiley & Sons, Ltd.     

Laser Interference Lithography for the Nanofabrication of Stimuli‐Responsive Bragg Stacks

Dynamic structural coloration in Tmesisternus isabellae beetle elytra is a unique example of Bragg stack‐based wavelength tuning in response to external stimuli. The underlying principles could guide the design of quantitative optical stimuli‐responsive polymers. Existing nanofabrication techniques to create such materials are costly, time‐consuming, and require high expertise. This study reports a nanofabrication method to produce slanted Bragg stack structures in poly(acrylamide‐co‐poly(ethylene glycol) diacrylate) hydrogel films by combining laser interference lithography and silver halide chemistry in a cost‐effective and rapid process (≈10 min). The Bragg stacks consist of silver bromide nanocrystal multilayers having a lattice spacing of ≈200 nm. Upon broadband light illumination, the Bragg stacks diffract a narrow‐band peak at 520 nm at ≈10° with respect to the normal incidence. The lattice spacing of the hydrogel films can be modulated by external stimuli to shift the Bragg peak for dynamic quantitative measurements. To demonstrate the utility of this method, the Bragg stacks are functionalized with phenylboronic acid molecules. Bragg peak shift analysis allows reversible glucose sensing within a physiological dynamic range (0.0–20.0 mmol L^?1) having a sensitivity of 0.2 mmol L^?1. The developed Bragg stacks may have application in portable, wearable, and implantable real‐time medical diagnostics at point‐of‐care settings.     

Multifunctional Core/Shell Nanoparticles Self‐Assembled from pH‐Induced Thermosensitive Polymers for Targeted Intracellular Anticancer Drug Delivery

Core/shell nanoparticles that display a pH‐sensitive thermal response, self‐assembled from the amphiphilic tercopolymer, poly(N‐isopropylacrylamide‐co‐N,N‐dimethylacrylamide‐co‐10‐undecenoic acid) (P(NIPAAm‐co‐DMAAm‐co‐UA)), have recently been reported. In this study, folic acid is conjugated to the hydrophilic segment of the polymer through the free amine group (for targeting cancer cells that overexpress folate receptors) and cholesterol is grafted to the hydrophobic segment of the polymer. This polymer also self‐assembles into core/shell nanoparticles that exhibit pH‐induced temperature sensitivity, but they possess a more stable hydrophobic core than the original polymer P(NIPAAm‐co‐DMAAm‐co‐UA) and a shell containing folate molecules. An anticancer drug, doxorubicin (DOX), is encapsulated into the nanoparticles. DOX release is also pH‐dependent. DOX molecules delivered by P(NIPAAm‐co‐DMAAm‐co‐UA) and folate‐conjugated P(NIPAAm‐co‐DMAAm‐co‐UA)‐g‐cholesterol nanoparticles enter the nucleus more rapidly than those transported by P(NIPAAm‐co‐DMAAm)‐b‐poly(lactide‐co‐glycolide) nanoparticles, which are not pH sensitive. More importantly, these nanoparticles can recognize folate‐receptor‐expressing cancer cells. Compared to the nanoparticles without folate, the DOX‐loaded nanoparticles with folate yield a greater cellular uptake because of the folate‐receptor‐mediated endocytosis process, and, thus, higher cytotoxicity results. These multifunctional polymer core/shell nanoparticles may make a promising carrier to target drugs to cancer cells and release the drug molecules to the cytoplasm inside the cells.     

Original Fuel‐Cell Membranes from Crosslinked Terpolymers via a “Sol–gel” Strategy

Hybrid organic/inorganic membranes that include a functionalized (‐SO₃H), interconnected silica network, a non‐porogenic organic matrix, and a ‐SO₃H‐functionalized terpolymer are synthesized through a sol–gel‐based strategy. The use of a novel crosslinkable poly(vinylidene fluoride‐ter‐perfluoro(4‐methyl‐3,6‐dioxaoct‐7‐ene sulfonyl fluoride)‐ter‐vinyltriethoxysilane) (poly(VDF‐ter‐PFSVE‐ter‐VTEOS)) terpolymer allows a multiple tuning of the different interfaces to produce original hybrid membranes with improved properties. The synthesized terpolymer and the composite membranes are characterized, and the proton conductivity of a hybrid membrane in the absence of the terpolymer is promising, since 8 mS cm^?1 is reached at room temperature, immersed in water, with an experimental ion‐exchange‐capacity (IEC_exp) value of 0.4 meq g^?1. Furthermore, when the composite membranes contain the interfaced terpolymer, they exhibit both a higher proton conductivity (43 mS cm^?1 at 65 °C under 100% relative humidity) and better stability than the standard hybrid membrane, arising from the occurrence of a better interface between the inorganic silica and the poly[(vinylidene fluoride)‐co‐hexafluoropropylene] (poly(VDF‐co‐HFP)) copolymer network. Accordingly, the hybrid SiO₂‐SO₃H/terpolymer/poly(VDF‐co‐HFP) copolymer membrane has potential use as an electrolyte in a polymer‐electrolyte‐membrane fuel cell operating at intermediate temperatures.     

Non‐volatile Ferroelectric Poly(vinylidene fluoride‐co‐trifluoroethylene) Memory Based on a Single‐Crystalline Tri‐isopropylsilylethynyl Pentacene Field‐Effect Transistor

A new type of nonvolatile ferroelectric poly(vinylidene fluoride‐co‐trifluoroethylene) (P(VDF‐TrFE)) memory based on an organic thin‐film transistor (OTFT) with a single crystal of tri‐isopropylsilylethynyl pentacene (TIPS‐PEN) as the active layer is developed. A bottom‐gate OTFT is fabricated with a thin P(VDF‐TrFE) film gate insulator on which a one‐dimensional ribbon‐type TIPS‐PEN single crystal, grown via a solvent‐exchange method, is positioned between the Au source and drain electrodes. Post‐thermal treatment optimizes the interface between the flat, single‐crystalline ab plane of TIPS‐PEN and the polycrystalline P(VDF‐TrFE) surface with characteristic needle‐like crystalline lamellae. As a consequence, the memory device exhibits a substantially stable source–drain current modulation with an ON/OFF ratio hysteresis greater than 10³, which is superior to a ferroelectric P(VDF‐TrFE) OTFT that has a vacuum‐evaporated pentacene layer. Data retention longer than 5 × 10⁴ s is additionally achieved in ambient conditions by incorporating an interlayer between the gate electrode and P(VDF‐TrFE) thin film. The device is environmentally stable for more than 40 days without additional passivation. The deposition of a seed solution of TIPS‐PEN on the chemically micropatterned surface allows fabrication arrays of TIPS‐PEN single crystals that can be potentially useful for integrated arrays of ferroelectric polymeric TFT memory.     

Light‐Induced Swelling‐Responsive Conductive,Adhesive, and Stretchable Wireless Film Hydrogel as Electronic Artificial Skin

Light‐induced wireless soft electronic skin hydrogels with excellent mechanical and electronic properties are important for several applications, such as soft robotics and intelligent wearable devices. Precise control of reversible stretchability and capacitive properties depending on intermolecular interaction and surface characteristics remains a challenge. Here, a thin‐film hydrogel is designed based on titanium oxide (TiO₂) polydopamine–perfluorosilica carbon dot‐conjugated chitosan–polyvinyl alcohol‐loaded tannic acid with controllable hydrophobic–hydrophilic transition in the presence of UV–vis light irradiation. The shifting of surface wettability from hydrophobic to hydrophilic by irradiation affects thin‐film water permeability and swelling ratio. This allows the penetration of water into the matrix to change its mechanical strength, electronic properties, and adhesive behavior. Specifically, the hydrogel displays mechanical strain as high as 278% in response to light stimuli and demonstrates the ability to regain its initial state determining the elasticity of the fabricated material. Moreover, the thin‐film hydrogel shows an increase in conductivity to 1.096 × 10^?3 and 1.026 × 10^?3 S cm^?1 when irradiated with UV and visible light, respectively. The hydrogel exhibits capacitive reversibility that follows finger motion which can be identified directly or remotely using wireless connection, indicative of its possible applications as an artificial electronic skin.