Photoresponsive Protein–Graphene–Protein Hybrid Capsules with Dual Targeted Heat‐Triggered Drug Delivery Approach for Enhanced Tumor Therapy

A novel photo‐responsive protein–graphene–protein (PGP) capsule that doubles as a photothermal agent with core/shell structure is constructed by anchoring reduced graphene oxide nanosheets on one‐component protein (lactoferrin) shell through a double emulsion method. PGP capsules can transport fully concealed hydrophilic anticancer cargo, doxorubicin (Dox), with a large payload (9.43 μmol g^‐1) to be later unloaded in a burst‐like manner by photo‐actuation triggered by near‐infrared irradiation. Being biocompatible yet with a high cancer cell targeting efficiency, PGP capsules have successfully eradicated subcutaneous tumors in 10 d following a single 5 min NIR irradiation without distal damage. Besides, the photochemothermal therapy of PGP capsules eradicates tumor cells not only in the light‐treating area but also widely light‐omitted tumor cells, overcoming the tumor recurrence due to efficient cell killing efficacy. These results demonstrate that the PGP capsule is a potential new drug delivery platform for local‐targeting, on‐demand, photoresponsive, combined chemotherapy/hyperthermia for tumor treatment and other biomedical applications.     

Photo‐ and pH‐Triggered Release of Anticancer Drugs from Mesoporous Silica‐Coated Pd@Ag Nanoparticles

A smart drug delivery system integrating both photothermal therapy and chemotherapy for killing cancer cells is reported. The delivery system is based on a mesoporous silica‐coated Pd@Ag nanoplates composite. The Pd@Ag nanoplate core can effectively absorb and convert near infrared (NIR) light into heat. The mesoporous silica shell is provided as the host for loading anticancer drug, doxorubicin (DOX). The mesoporous shell consists of large pores, ～10 nm in diameter, and allows the DOX loading as high as 49% in weight. DOX loaded core–shell nanoparticles exhibit a higher efficiency in killing cancer cells than free DOX. More importantly, DOX molecules are loaded in the mesopores shell through coordination bonds that are responsive to pH and heat. The release of DOX from the core‐shell delivery vehicles into cancer cells can be therefore triggered by the pH drop caused by endocytosis and also NIR irradiation. A synergistic effect of combining chemotherapy and photothermal therapy is observed in our core‐shell drug delivery system. The cell‐killing efficacy by DOX‐loaded core–shell particles under NIR irradiation is higher than the sum of chemotherapy by DOX‐loaded particles and photothermal therapy by core–shell particles without DOX.     

Responsive Macroscopic Materials From Self‐Assembled Cross‐Linked SiO2‐PNIPAAm Core/Shell Structures

A way to obtain macroscopic responsive materials from silicon‐oxide polymer core/shell microstructures is presented. The microparticles are composed of a 60 nm SiO₂‐core with a random copolymer corona of the temperature responsive poly‐N‐isopropylacrylamide (PNIPAAm) and the UV‐cross‐linkable 2‐(dimethyl maleinimido)‐N‐ethyl‐acrylamide. The particles shrink upon heating and form a stable gel in both water and tetrahydrofuran (THF) at 3–5 wt% particle content. Cross‐linking the aqueous gel results in shrinkage when the temperature is increased above the lower critical solution temperature and it regains its original size upon cooling. By freeze drying with subsequent UV irradiation, thin stable layers are prepared. Stable fibers are produced by extruding a THF gel into water and subsequent UV irradiation, harnessing the cononsolvency effect of PNIPAAm in water/THF mixtures. The temperature responsiveness translates to the macroscopic materials as both films and fibers show the same collapsing behavior as the microcore/shell particle. The collapse and re‐swelling of the materials is related to the expelling and re‐uptake of water, which is used to incorporate gold nanoparticles into the materials by a simple heating/cooling cycle. This allows for future applications, as various functional particles (antibacterial, fluorescence, catalysis, etc.) can easily be incorporated in these systems.     

pH‐Responsive Peptide Mimic Shell Cross‐Linked Magnetic Nanocarriers for Combination Therapy

The design and development of water dispersible, pH responsive peptide mimic shell cross‐linked magnetic nanocarriers (PMNCs) using a facile soft‐chemical approach is reported. These nanocarriers have an average size about 10 nm, are resistant to protein adsorption in physiological medium, and transform from a negatively charged to a positively charged form in the acidic environment. The terminal amino acid on the shell of the magnetic nanocarriers allows us to create functionalized exteriors with high densities of organic moieties (both amine and carboxyl) for conjugation of drug molecules. The drug‐loading efficiency of the nanocarriers is investigated using doxorubicin hydrochloride (DOX) as a model drug to evaluate their potential as a carrier system. Results show high loading affinity of nanocarriers for anticancer drug, their sustained release profile, magnetic‐field‐induced heating, and substantial cellular internalization. Moreover, the enhanced toxicity to tumor cells by DOX‐loaded PMNCs (DOX‐PMNCs) under an AC magntic field suggest their potential for combination therapy involving hyperthermia and chemotherapy.     

Near‐Infrared Triggered Release of uPA from Nanospheres for Localized Hyperthermia‐Enhanced Thrombolysis

Currently, most thrombolytic agents are limited by short circulation time and excessive dose needed for clinical therapy, which increases lethal risk for intracranial hemorrhage. Here, a near‐infrared‐triggered, controlled‐release system, using gold@mesoporous silica core–shell nanospheres (Au@MSNs) with phase‐changed material 1‐tetradecanol, is formulated to release urokinase plasminogen activators (uPA) on demand. The prepared system presents a sensitive system for releasing uPA, owing to an elevated temperature created by Au@MSNs‐induced photothermal effect. For in vitro study, a 3D printed vein vasculature is designed and fabricated to simulate the thrombolysis of system in blood vessel. Murine tail thrombus model is also built to evaluate thrombolysis in vivo. Consequently, localized hyperthermia is validated to possess an effective enhancement for thrombolysis. Therefore, according to the results, the fabricated system demonstrates two aspects of potential superiority: controlled uPA release for reducing risk of side effects, and hyperthermia‐enhanced thrombolysis locally for decreasing drug dosage. Assisted with thermal thrombolysis, the present formulated system shows a high efficiency, on‐demand drug release, and thus a safer protocol for thrombolytic therapy, which fits the developing trends of precision medicine.     

Highly Efficient Diels–Alder Crosslinkable Electro‐Optic Dendrimers for Electric‐Field Sensors

One of the most challenging tasks encountered in developing highly efficient electro‐optic (EO) devices is to find a material system that possesses all desirable properties such as large EO coefficients, good thermal and mechanical stability, and low optical loss. In order to meet this stringent requirement, we have developed a series of crosslinkable EO dendrimers using the standardized AJL8 ‐type chromophore as the center core and the furyl‐ and anthryl‐containing dendrons as the periphery. Upon adding a trismaleimide ( TMI ) dienophile, these dendrimers could be in‐situ crosslinked via the Diels–Alder cycloaddition and efficiently poled under a high electric field. Through this dynamic process, the spatially voided and π‐electron‐rich surrounding of the chromophore core changes into a dense and more aliphatic network, with the dipolar chromophore embedded and aligned inside. The resultant materials exhibit large EO coefficients (63–99 pm V^–1 at 1.31 μm), excellent temporal stability (the original r₃₃ values remain unchanged at 100 °C for more than 500 h), and blue‐shifted near‐IR absorption. With these combined desirable properties, a poled EOD2/TMI film could be processed through multiple lithographic and etching steps to fabricate a racetrack‐shaped micro‐ring resonator. By coupling this ring resonator with a side‐polished optical fiber, a novel broadband electric‐field sensor with high sensitivity of 100 mV m^–1 at 550 MHz was successfully demonstrated.     

Temperature‐Switchable Assembly of Supramolecular Virus–Polymer Complexes

Here a method is presented for the temperature‐switchable assembly of viral particles into large hierarchical complexes. Dual‐functional diblock copolymers consisting of poly(diethyleneglycol methyl ether methacry­late) (poly(DEGMA)) and poly((2‐dimethylamino)ethyl methacrylate) (poly(DMAEMA)) blocks self‐assemble electrostatically with cowpea chlorotic mottle virus (CCMV) particles into micrometer‐sized objects as a function of temperature. The poly(DMAEMA) block carries a positive charge, which can interact electrostatically with the negatively charged outer surface of the CCMV capsid. When the solution temperature is increased above 40 °C, to cross the cloud point temperature (T_cp) of the DEGMA block, the polymer chains collapse on the surface of the virus particle, which makes them partially hydrophobic, and consequently causes the formation of large hierarchical assemblies. Disassembly of the virus–polymer complexes can be induced by reducing the solution temperature below the T_cp, which allows the poly(DEGMA) blocks to rehydrate and free virus particles to be released. The assembly process is fully reversible and can sustain several heating–cooling cycles. Importantly, this method relies on reversible supramolecular interactions and therefore avoids the irreversible covalent modification of the particle surface. This study illustrates the potential of temperature‐responsive polymers for controlled binding and releasing of virus particles.     

Zwitterionic Polysulfamide Drug Nanogels with Microwave Augmented Tumor Accumulation and On‐Demand Drug Release for Enhanced Cancer Therapy

Zwitterionic polymers demonstrate as a class of antifouling materials with long blood circulation in living subjects. Despite extensive research on their antifouling abilities, the responsive zwitterionic polymers that can change their properties by mild outside signals are poorly explored. Herein, a sulfamide‐based zwitterionic monomer is developed and used to synthesize a series of polysulfamide‐based (poly (2‐((2‐(methacryloyloxy)ethyl) dimethylammonio)acetyl) (phenylsulfonyl) amide (PMEDAPA)) nanogels as drug carriers for effective cancer therapy. PMEDAPA nanogels are proved to exhibit prolonged blood circulation without inducing the accelerated blood clearance phenomenon. Intriguingly, PMEDAPA nanogels can sensitively respond to hyperthermia by adjusting the crosslinker degree. After modified with transferrin (Tf), the nanogels (PMEDAPA‐Tf) achieve shielded tumor targeting at normothermia, while exhibiting recovered tumor targeting at hyperthermia, leading to enhanced tumor accumulation. Meanwhile, PMEDAPA‐Tf nanogels show superior penetration ability in 3D tumor spheroids and faster drug release at hyperthermia compared with that at normothermia. In combination with mild microwave heating (≈41 °C), the drug‐loaded PMEDAPA‐Tf nanogels show a pronounced tumor inhibition effect in a humanized orthotropic liver cancer model. Therefore, the study provides a novel hyperthermia‐responsive zwitterionic nanogel that can achieve augmented tumor accumulation and on‐demand drug release assisted with clinically used microwave heating for cancer therapy.     

Formation Mechanism of Epitaxial Palladium–Platinum Core–Shell Nanocatalysts in a One‐Step Supercritical Synthesis

The scarcity of platinum group metals provides a strong incentive to optimize the catalytic activity and stability, e.g., through nanoalloys or core–shell nanoparticles. Here, time‐resolved X‐ray total scattering and transmission electron microscopy characterization are used to study the formation of palladium–platinum core–shell nanoparticles under solvothermal conditions. It is shown that Pd rapidly forms small (5–10 nm), disordered primary particles, which agglomerate and crystallize when reaching 20–25 nm. The primary Pd particles provide nucleation sites for Pt, and, with extended reaction time, the Pd cores become fully covered with Pt shells. The observed core–shell material is surprising when considering the Pt–Pd phase diagram and relative surface energies, but it can be rationalized through the kinetics of precursor conversion. To bridge the gap between scientific studies and industrial demand for large‐scale production, the synthesis process is successfully transferred to a continuous flow supercritical reactor providing a simple scalable and green process for production of bimetallic nanocatalysts.     

CCVD Synthesis of Carbon‐Encapsulated Cobalt Nanoparticles for Biomedical Applications

Carbon‐encapsulated ferromagnetic Cobalt nanoparticles (Co@C) have been synthesized by catalytic chemical vapour deposition (CCVD). The nanoparticles, mainly ranging between 10 and 15 nm, are tightly encapsulated by 2–3 concentric graphitic carbon shells and protected from oxidation. Because of their magnetic properties (saturation magnetization of 106 emu/g and a coercivity HC of 250 Oe), Co@C nanoparticles have been investigated for hyperthermia application. Although the observed values of the specific absorption rate (28.7 W/gCo@C at 30 kA/m and 215.4 W/gCo@C at 70 kA/m) are slightly lower than required in actual hyperthermia therapies, the observed strong heating effect provides a very promising starting point for future clinical application. It is also demonstrated that these nanoparticles can at the same time be used for magnetic resonance imaging (MRI) with an efficiency comparable to commercially available T2 contrast agents.     

Laser‐Induced In‐Fiber Fluid Dynamical Instabilities for Precise and Scalable Fabrication of Spherical Particles

Scalable fabrication of spherical particles at both the micro‐ and nanoscales is of significant importance for applications spanning optical devices, electronics, targeted drug delivery, biodevices, sensors, and cosmetics. However, current top‐down and bottom‐up fabrication methods are unable to provide the full spectrum of uniformly sized, well‐ordered, and high‐quality spheres due to their inherent restrictions. Here, a generic, scalable, and precisely controllable fabrication method is demonstrated for generating spherical particles in a full range of diameters from microscale to nanoscale. This method begins with a macroscopic composite multimaterial solid‐state preform drawn into a fiber that defines precisely the initial conditions for the process. It is then followed by CO₂ laser heating to enable the transformation from a continuous fiber core into a series of homogeneous spheres via Plateau–Rayleigh capillary instability inside the fiber. This physical breakup method applies to a wide range of functional materials with different melting temperatures from 400 to 2400 K and 10 orders of difference in fiber core/cladding viscosity ratio. Furthermore, an ordered array of silicon‐based whispering‐gallery mode resonators with the Q factor as high as 7.1 × 10⁵ is achieved, owing to the process induced ultrasmooth surface and highly crystalline nature.     

The Development of Yolk–Shell‐Structured Pd&ZnO@Carbon Submicroreactors with High Selectivity and Stability

Design of multicomponent yolk–shell structures is crucial for the fabrication of micro/nanoreactors for a variety of applications. This work reports the rational design and synthesis of yolk–shell‐structured submicroreactors with loaded metal nanoparticles into ZnO–microporous carbon core–shell structures. The solvothermal treatment and carbonization process of uniform zeolitic imidazolate framework‐8 (ZIF‐8)@resin polymer core–shell structures leads to the generation of yolk–shell‐structured ZnO@carbon. The synthesis conditions are optimized to track the evolution of ZIF‐8 in a confined space of resin polymer as a submicroreactor itself. It is found that nanoribbon evolution occurs via the formation of the intermediate needle‐like particles. The Pd&ZnO@carbon submicroreactor is shown to be a highly selective catalyst (selectivity >99%) for hydrogenation of phenylacetylene to phenylethylene. The excellent performance of Pd&ZnO@carbon particles is evidenced by higher conversion and selectivity than that of Pd/ZnO and Pd/C with similar Pd loading. Furthermore, Pd&ZnO@carbon submicroreactors show superior catalytic stability, and no deactivation after 25 h of reaction. The proposed strategy is promising for the design of multifunctional micro/nanoreactors or nanocontainers for construction of artificial cells.     

Biopebbles: DNA‐Functionalized Core–Shell Silica Nanospheres for Cellular Uptake and Cell Guidance Studies

The development of a versatile class of silica nanoparticles for cell studies is reported. The particles contain a fluorescent dye‐encoded core and a single‐stranded DNA oligonucleotide‐displaying shell. They are accessible in arbitrary size and color through robust protocols for Stöber‐based colloidal synthesis and sturdy chemical surface functionalization. Silica particles in the size range of 100 nm to 1.5 µm diameter containing fluorescein, Cy3 oder Cy5 dye‐encoded cores are synthesized and functionalized with DNA oligonucleotides. These silica biopebbles are conveniently traceable by microscopy and have a high affinity to live cells, which makes them ideal for cell uptake studies, as demonstrated for MCF7 and A431 cancer cells. The biopebbles can be utilized as building blocks for the self‐assembled formation of arbitrary surface patterns on glass substrates. With these architectures, the privileged internalization of the biopebbles can be exploited for improved adhesion and guidance of cells because the particles are no longer ingested by adhered cells due to their physical connection with the solid support. It is believed that the biopebble approach will be useful for a variety of applications, fundamental studies in cell biology and tissue engineering.     

Magnetic Hyperthermia–Synergistic H2O2 Self‐Sufficient Catalytic Suppression of Osteosarcoma with Enhanced Bone‐Regeneration Bioactivity by 3D‐Printing Composite Scaffolds

Chemotherapy resistance and bone defects caused by surgical excision of osteosarcoma have been formidable challenges for clinical treatment. Although recently developed nanocatalysts based on Fenton‐like reactions for catalytic therapy demonstrate high potential to eliminate chemotherapeutic‐insensitive tumors, insufficient concentration of intrinsic hydrogen peroxide (H₂O₂) and low intratumoral penetrability hinder their applications and therapeutic efficiency. The synchronous enriching intratumor H₂O₂ amount or nanoagents and promoting osteogenesis are intriguing strategies to solve the dilemma in osteosarcoma therapy. Herein, a multifunctional “all‐in‐one” biomaterial platform is constructed by co‐loading calcium peroxide (CaO₂) and iron oxide (Fe₃O₄) nanoparticles into a three‐dimensional (3D) printing akermanite scaffold (AKT‐Fe₃O₄‐CaO₂). The loaded CaO₂ nanoparticles act as H₂O₂ sources to achieve H₂O₂ self‐sufficient nanocatalytic osteosarcoma therapy as catalyzed by coloaded Fe₃O₄ nanoagents, as well as provide calcium ion (Ca²⁺) pools to enhance bone regeneration. The synergistic osteosarcoma‐therapeutic effect is achieved from both magnetic hyperthermia as‐enabled by Fe₃O₄ nanoparticles under alternative magnetic fields and hyperthermia‐enhanced Fenton‐like nanocatalytic reaction for producing highly toxic hydroxyl radicals. Importantly, the constructed 3D AKT‐Fe₃O₄‐CaO₂ composite scaffolds are featured with favorable bone‐regeneration activity, providing a worthy base and positive enlightenment for future osteosarcoma treatment with bone defects by the multifunctional biomaterial platforms.     

Synthesis of Au–CdS Core–Shell Hetero‐Nanorods with Efficient Exciton–Plasmon Interactions

The synthesis of large lattice mismatch metal‐semiconductor core–shell hetero‐nanostructures remains challenging, and thus the corresponding optical properties are seldom discussed. Here, we report the gold‐nanorod‐seeded growth of Au–CdS core–shell hetero‐nanorods by employing Ag₂S as an interim layer that favors CdS shell formation through a cation‐exchange process, and the subsequent CdS growth, which can form complete core–shell structures with controllable shell thickness. Exciton–plasmon interactions observed in the Au–CdS nanorods induce shell thickness‐tailored and red‐shifted longitudinal surface plasmon resonance and quenched CdS luminescence under ultraviolet light excitation. Furthermore, the Au–CdS nanorods demonstrate an enhanced and plasmon‐governed two‐photon luminescence under near‐infrared pulsed laser excitation. The approach has potential for the preparation of other metal‐semiconductor hetero‐nanomaterials with complete core–shell structures, and these Au–CdS nanorods may open up intriguing new possibilities at the interface of optics and electronics.     

The Effects of Embedded Dipoles in Aromatic Self‐Assembled Monolayers

Using a representative model system, here electronic and structural properties of aromatic self‐assembled monolayers (SAMs) are described that contain an embedded, dipolar group. As polar unit, pyrimidine is used, with its orientation in the molecular backbone and, consequently, the direction of the embedded dipole moment being varied. The electronic and structural properties of these embedded‐dipole SAMs are thoroughly analyzed using a number of complementary characterization techniques combined with quantum‐mechanical modeling. It is shown that such mid‐chain‐substituted monolayers are highly interesting from both fundamental and application viewpoints, as the dipolar groups are found to induce a potential discontinuity inside the monolayer, electrostatically shifting the core‐level energies in the regions above and below the dipoles relative to one another. These SAMs also allow for tuning the substrate work function in a controlled manner independent of the docking chemistry and, most importantly, without modifying the SAM‐ambient interface.     

Doxorubicin‐Loaded Single Wall Nanotube Thermo‐Sensitive Hydrogel for Gastric Cancer Chemo‐Photothermal Therapy

Single wall carbon nanotube (SWNT) based thermo‐sensitive hydrogel (SWNT‐GEL) is reported, which provides an injectable drug delivery system as well as a medium for photothermal transduction. SWNT‐hydrogel alone appears to be nontoxic on gastric cancer cells (BGC‐823 cell line) but leads to cell death with NIR radiation through a hyperthermia proapoptosis mechanism. By incorporating hyperthermia therapy and controlled in situ doxorubicin (DOX) release, DOX‐loaded SWNT‐hydrogel with NIR radiation proves higher tumor suppression rate on mice xenograft gastric tumor models compared to free DOX without detectable organ toxicity. The developed system demonstrates improved efficacy of chemotherapeutic drugs which overcomes systemic adverse reactions and presents immense potential for gastric cancer treatment.     

Polyaniline–Silica Composite Conductive Capsules and Hollow Spheres

In this paper, we report on the preparation of monodisperse polyaniline (PANi)–silica composite capsules and hollow spheres on monodisperse core–gel‐shell template particles. An extension of the previously reported inward growth method was used. The samples were self‐stabilized without external additives. The core–gel‐shell particles were prepared by the inward sulfonation of monodisperse polystyrene particles. The introduced sulfonic acid and sulfone groups are responsible for the gel properties. The gel‐shell thickness and core size were synchronously controlled over the whole particle radius range. After aniline (ANi) monomer was preferentially absorbed in the sulfonated polystyrene shell, PANi was formed by polymerization. PANi was doped in situ with a sulfonic acid group to give the capsules a high conductivity. PANi hollow spheres were derived after the polystyrene cores were dissolved: their cavity size and shell thickness were synchronously controlled by using different core–gel‐shell particles. The PANi–silica composite capsules and hollow spheres were therefore prepared by a sol–gel process using tetraethylorthosilicate in the conducting shell. The PANi shell became more robust while maintaining the same conductivity level. Morphological results indicate that the PANi and silica formed a bicontinuous network. Fourier‐transform infrared (FTIR) spectra revealed that the hydrogen bonding in the PANi–gel shell was enhanced after the silica phase was incorporated, which could explain the high conductivity level after the silica phase was added. In a converse procedure, silica capsules and hollow spheres were prepared by a sol–gel process that incorporated tetraethylorthosilicate into the core–gel‐shell templates, which was followed by the absorption and polymerization of aniline in the silica shell thus forming PANi–silica composite capsules and hollow spheres. The silica capsules and hollow spheres thereby became conductive.     

Two‐Dimensional Assembly of Symmetric Colloidal Dimers under Electric Fields

Like atoms and molecules with directional interactions, anisotropic particles could potentially assemble into a much wider range of crystalline arrays and meso‐structures than spherical particles with isotropic interactions. In this paper, the electric‐field directed assembly of geometrically anisotropic particles–colloidal dimers is studied. Rich phase behavior and different assembly regimes are found, primarily arising from the broken radial symmetry in particles. The orientations of individual dimers depend on the frequency of the electric field, the ramping direction of frequency, and the salt concentration. The competition and balance between the hydrodynamic, electric, and Brownian torques determine the orientation of individual particles, while the competition between the electrohydrodynamic force and dipolar interaction determines the aggregation of aligned particles at a given experimental condition. The field distribution near the electrode is critical to understand the orientation and assembly behavior of colloidal dimers on a conducting substrate. This study also demonstrates the effectiveness, the reversibility, and potential opportunity of applying electric field to control the orientation and direct the assembly of non‐spherical particles. In particular, two dimensional close‐packed crystals of perpendicularly aligned dimers are obtained, which shows promise in fabricating 3D photonic crystals based on dimer‐like colloids and field‐directed display.     

Mesostructured Nonwovens with Penguin Downy Feather‐Like Morphology—Top‐Down Combined with Bottom‐Up

Polymer fibers play an important role in nature and technical systems. Fiber morphologies with off‐standing branches, as found in nature, e.g. in penguin downy feathers, provide unique properties but are unknown for man‐made polymer fiber systems. We discovered that it is possible to initiate seeded growth from trisamide seeded polystyrene fibers, prepared by core‐shell electrospinning, to form off‐standing supramolecular trisamide branches similar to penguin downy feathers but in polymer nonwovens and in nanoscale. Resulting mesostructured nonwovens show unique properties. For example, air filtration efficiency of 99.8% for the filtration of 0.3 µm aerosol particles, being significantly higher compared to neat electrospun polystyrene nonwovens as bench‐mark, showing only an efficiency of about 52.6%. Most remarkably, the pressure drop observed in filtration tests and thus, the energy consumption during filtration, did not increase up to a certain content of off‐standing supramolecular fibrils. This is a unique behavior, as higher filtration capabilities are typically connected to higher energy consumptions and pressure drops. Hence, branching electrospun fibers with supramolecular fibrils paves the way to new mesostructured nonwovens with unique morphologies, property profiles and applications in filtration, catalysis, and energy storage/harvesting, exploiting nature's concepts.