Collagen membranes possess ideal biological properties and can be served as a barrier for supporting infiltration and proliferation of osteoblasts in guided bone regeneration (GBR). However, pure collagen lacks desirable mechanical properties and also leads to inflammation, resulting in progressive bone resorption. In our previous study, EGCG cross-linked collagen membranes exhibit better mechanical properties and anti-inflammatory effect. However, higher concentration of EGCG may not improve cell viability. Herein, we present an enhanced EGCG cross-linked collagen membranes with surface modification of PEG to improve cell viability and cell adhesion, considering the better biocompatibility of PEG. Scanning electron microscope images showed that PEG-EGCG-collagen membrane exhibited smoother surface fiber aggregates. Fourier transform infrared spectroscopy demonstrated that the structure characteristics were maintained after addition of EGCG and PEG. Cell viability was significantly increased after modification of PEG, as determined by the Cell Counting Kit-8 (CCK-8) and live/dead assay. Better shapes of cytoskeleton were observed in immunostaining images. Additionally, enzyme-linked immunosorbent assay showed PEG-EGCG-collagen membrane significantly decreased the level of inflammatory factors secreted by MG63 cells. Collectively, with respect to all the aspects including intact structure, cell viability promotion and mediation of pro-inflammatory cytokine secretion, our results indicate that PEG-EGCG-collagen membrane might be used in GBR applications.