Biomacromolecules with poor mechanical properties cannot satisfy the stringent requirement for load-bearing as bioscaffolds. Herein, we proposed to develop a biodegradable high-strength supramolecular polymer strengthened biomacromolecules-based hydrogel composed of cleavable poly(N-acryloyl 2-glycine) (PACG) and methacrylated gelatin (GelMA) (PACG-GelMA) and further fabricated the biohybrid gradient scaffold for osteochondral regeneration by a 3D printing technique. In vitro and in vivo experiments demonstrate that the constructed scaffold can simultaneously promote the regeneration of both cartilage and subchondral bone within osteochondral defects, offering a promising strategy for osteoarthritis treatment.