Polycaprolactone (PCL) scaffolds with a honeycomb (hc) microstructure have been prepared, modified at surface level by plasma processes and evaluated with human mesenchymal stem cells (hMSCs). Thin scaffolds were fabricated by self‐assembly of PCL in the presence of an amphiphilic copolymer under controlled humidity. The surface of the so formed PCLhc scaffolds was modified by Ar and ArO2 plasma discharges and by plasma deposition of allylamine (ALA). Such modification induces composition changes and microstructure modifications as determined by Fourier transformed infrared spectroscopy and scanning electron microscopy. As a consequence of these treatments, the hydrophobic character of PCLhc scaffolds is rectified as derived from water contact angle measurements. The hMSC cytocompatibility of these scaffolds was initially assayed under proliferation conditions evaluating surface–cell interactions by fluorescence and confocal microscopy. Most relevant behaviour was observed for hMSCs cultured onto ALA modified scaffolds in view of the cytoskeleton polarization. These modified surfaces were further explored for differentiation of hMSCs in the presence of vitamin D, giving rise to secreting vesicles and increased extension of the cytoskeleton. These results are promising for the development of cell monolayer tissue regenerating platforms.

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aThe current work describes a hydrogel route for the amine functionalization of polycaprolactone scaffolds with a honeycomb structure (PCLhc). The functionalization takes place after contact with fresh liquid hydrogels. After gelification, hydrogels are removed for evaluation of the transferred active molecules. The formation of hybrids with variable agarose/aminopropyltriethoxysilane (APTS) ratio allowing gradual grafting was evaluated initially onto Si planar surfaces. Analysis of the line shape of Si 2p XPS allowed confirming on the one hand that Si-O x contribution related to APTS increases as Si-Si signal due to Si (100) substrate decreases for increasing aminosilane load in the gel. On the other hand, the line shape of C 1s and N 1s core level spectra were characteristic of those related to APTS functionalization, with a particular label due to partial agarose transfer to the substrate. In this stage, PCLhc scaffolds were activated with the agarose-APTS hybrids. A peeling after gelification gave rise not only to amine-activated PCLhc structures, but also to hc structure replicas on the contacting surfaces of the agarose-APTS hydrogels. In order to evaluate the activity of modified PCLhc scaffolds, a labeled mouse antibody was immobilized and its functionalization evaluated by fluorescence microscopy.