Poly(gallic acid), a novel polymer obtained by enzymatic polymerization of gallic acid, was successfully cross-linked to carboxymethylcellulose using citric acid as a cross-linker. Non-woven sheets were prepared with the resulting copolymer and their in vitro biocompatibility was assessed. The results on the characterizations of the produced films by mechanical tests, water vapour permeability, contact angle, and antioxidant activity by electronic paramagnetic resonance were adequate for skin tissue regeneration. Films were also decomposed under physiological conditions using universal buffers at pH 3, 7 and 10. In vitro experiments with fibroblast-like and epithelial-like cells showed good adhesion and proliferation onto the PGAL-co-CMC sheets. These non-woven sheets can consequently be considered as novel biocompatible and biodegradable films with high-responsiveness for biomedical or tissue engineering applications.