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An ideal synthetic bone graft is a combination of the porous and nanofibrous structure presented by natural bone tissue as well as osteoinductive biochemical factors such as bone morphogenetic protein 2 (BMP‐2). In this work, ultralight 3D hybrid nanofiber aerogels composed of electrospun PLGA‐collagen‐gelatin and Sr–Cu codoped bioactive glass fibers with incorporation of heptaglutamate E7 domain specific BMP‐2 peptides have been developed and evaluated for their potential in cranial bone defect healing. The nanofiber aerogels are surgically implanted into 8 mm × 1 mm (diameter × thickness) critical‐sized defects created in rat calvariae. A sustained release of E7‐BMP‐2 peptide from the degradable hybrid aerogels significantly enhances bone healing and defect closure over 8 weeks in comparison to unfilled defects. Histomorphometry and X‐ray microcomputed tomography (µ‐CT) analysis reveal …