3D-Printable biomaterials have potential for fabrication of customized scaffolds for tissue engineering. In the study, methacrylated gelatin (GelMA) and aldehyde-functionalized polyurethane (PU) were synthesized and used to prepare 3D-printable GelMA-PU biomaterials. The GelMA-PU hydrogel and cryogel were optimized for compositions and manufacture processes. The GelMA-PU hydrogel was 3D-printable through a 210 µm nozzle. The separately printed modules could be further assembled into constructs of complex structure owing to the self-healing ability, and the integrated structure was stabilized by secondary photo-crosslinking. The self-healing ability of the hydrogel was switched off after photo-crosslinking while the resolution was maintained. The GelMA-PU hydrogel embedding human bone marrow mesenchymal stem cells (hMSCs) was successfully printed and grown for 14 days. Besides, 16-gauge needle injectable cryogel with high compressibility was acquired by adjusting the composition of GelMA/DFPU and freezing. The latter cryogel was 3D-printable through a programmed low-temperature printing procedure. The 3D-printed GelMA-PU cryogel scaffolds displayed high swelling ratio and remained the high compressibility. hMSCs seeded in the 3D-printed GelMA-PU cryogel scaffolds also displayed long-term growth in 14 days. The GelMA-PU composite systems demonstrate the versatility as both hydrogel and cryogel, which have potential applications in 3D bioprinting, tissue engineering, and minimally invasive surgery.