Gelatin-based hydrogel, which mimics the natural dermal extracellular matrix, is a promising tissue engineering material. However, insufficient and uncontrollable mechanical and degradation properties remain the major obstacles for its application in medical bone regeneration material. Herein, we develop a facile but efficient strategy for a novel hydrogel as guided bone regeneration (GBR) material. In this study, methacrylic anhydride (MA) has been used to modify gelatin to obtain photo-crosslinkable methacrylated gelatin (GelMA). Moreover, the GelMA/PEGDA hydrogel was prepared by photo-crosslinking GelMA and PEGDA with photoinitiator I2959 under UV treatment. Compared with the GelMA hydrogel, the GelMA/PEGDA hydrogel exhibits several times stronger mechanical properties than pure GelMA hydrogel. The GelMA/PEGDA hydrogel shows a suitable degradation rate of more than 4 weeks, which is beneficial to implant in body. In vitro cell culture showed that osteoblast can adhere and proliferate on the surface of the hydrogel, indicating that the GelMA/PEGDA hydrogel had good cell viability and biocompatibility. Furthermore, by changing the quantities of GelMA, I2959, and PEGDA, the gelation time can be controlled easily to meet the requirement of its applications. In short, this study demonstrated that PEGDA enhanced the performance and extended the applications of GelMA hydrogels, turning the GelMA/PEGDA hydrogel into an excellent GBR material.

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