In article 1701415, Jingwei Xie and co‐workers report the fabrication of novel three‐dimensional (3D) hybrid nanofiber aerogels composed of electrospun PLGA‐collagen‐gelatin (PCG) and Sr‐Cu co‐doped bioactive glass (BG) fiber segments, with incorporation of heptaglutamate E7 domain specific BMP‐2 peptides, through calcium binding. Their potential applications in healing a critical‐sized cranial bone defect is reported.