Development of Functional Coatings from Amphiphilic Polymer Co-networks with Enhanced Cell Adhesion

Functional coatings based on amphiphilic polymer co-networks (ACNs) offer a versatile alternative to hydrogel coatings in biomedical research, providing enhanced mechanical stability and a broad range of tunable properties. This study systematically explores ACN thin films composed of star-shaped poly(ε-caprolactone) (PCL) and poly(ethylene glycol) (PEG) with varying PEG content to identify coatings with optimized amphiphilic balance for cell adhesion. Films with low PEG content (9 and 15 wt-%) promote significant protein adsorption and cell attachment, whereas PEG-rich films (38 and 47 wt-%) exhibit negligible protein adsorption and effectively inhibit cell adhesion. An ultrathin decellularized and digested extracellular matrix (dECM) coating was used to restore cell adhesiveness on PEG-rich ACN films while preserving their intrinsic material characteristics. Fibroblast studies showed that stiffness and surface roughness modulate cellular metabolic activity but do not affect initial adhesion. Time-dependent cell numbers on the samples reached levels comparable to or exceeding those on tissue culture polystyrene controls. Drug-proxy uptake depended strongly on network composition, with the highest uptake of Lucifer Yellow in PCL10_PEG10 films (~180 ng cm-2) and markedly higher uptake of Nile Red (~10 µg cm-2). These findings demonstrate the potential of ACNs as versatile functional materials for biointerface engineering in the biomedical field.