Bioadhesives are becoming an essential and important ingredient in medical science. Despite numerous reports, developing adhesive materials that combine strong adhesion, biocompatibility, and biodegradation remains a challenging task. Here, we present a biocompatible yet biodegradable block copolymer-based waterborne superglue that leads to an application of follicle-free hair transplantation. Our design strategy bridges self-assembled, temperature-sensitive block copolymer nanostructures with tannic acid as a sticky and biodegradable polyphenolic compound. The formulation further uniquely offers step-by-step increases in adhesion strength via heating–cooling cycles. Combining the modular design with the thermal treating process enhances the mechanical properties up to 5 orders of magnitude compared to the homopolymer formulation. This study opens a new direction in bioadhesive formulation strategies utilizing block copolymer nanotechnology for systematic and synergistic control of the material’s properties.

We report self-assembly of a statistical copolymer poly(styrene-co-methyl methacrylate) (P(S-co-MMA)) containing ionic liquid (IL)-philic methyl methacrylate (MMA) and IL-phobic styrene (S) repeating units in IL for fabrication of electrolyte-gated organic transistors. P(S-co-MMA)s with high MMA contents were synthesized by copolymerization of styrene and MMA via a reversible addition–fragmentation chain transfer (RAFT) process, and their behavior in 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([EMI][TFSI]) was investigated. While dynamic light scattering analysis showed formation of a micellar solution at low concentration, the elastic modulus of the viscoelastic solution increased significantly more than the loss modulus at high concentration. Small angle X-ray scattering analysis suggested ill-defined phase separation between PS-rich segments and PS-lean segments swollen in [EMI][TFSI]. The resulting P(S-co-MMA)/[EMI][TFSI] mixture exhibited increased ionic conductivity compared to the PS-b-PMMA-b-PS block polymer gel, as well as superior device performance in transistor gating experiments.

We report a blending mechanism of polystyrene-b-poly(ethylene oxide) (PS-b-PEO) and PS homopolymer (homoPS) at the air/water interface. Our blending mechanism is completely different from the well-known “wet–dry brush theory” for bulk blends; regardless of the size of homoPS, the domain size increased and the morphology changed without macrophase separation, whereas the homoPS of small molecular weight (MW) leads to a transition after blending into the block copolymer domains, and the large MW homoPS is phase-separated in bulk. The difference in blending mechanism at the interface is attributed to adsorption kinetics at a water/spreading solvent interface. Upon spreading, PS-b-PEO is rapidly adsorbed to the water/spreading solvent interface and forms domain first, and then homoPS accumulates on them as the solvent completely evaporates. On the basis of our proposed mechanism, we demonstrate that rapid PS-b-PEO adsorption is crucial to determine the final morphology of the blends. We additionally found that spreading preformed self-assemblies of the blends slowed down the adsorption, causing them to behave similar to bulk blends, following the “wet–dry brush theory”. This new mechanism provides useful information for various block copolymer-homopolymer blending systems with large fluid/fluid interfaces such as emulsions and foams.