Pathological myopia (PM) is a leading cause of irreversible vision impairment, characterized by progressive axial elongation and posterior staphyloma. Posterior scleral reinforcement (PSR) surgery is a key intervention to halt disease progression. In this procedure, PSR materials are fixed to the posterior pole of the eye to enhance the original scleral biomechanical properties and promote collagen deposition. However, the materials used for PSR are difficult to obtain and fail to fully achieve all required biomechanical functions. In this study, a novel bilayered biomaterial combining mechanical support with bio-regenerative capacity was developed. The outer reinforcement layer was a decellularized porcine sclera (dPS), while the inner functional layer was a gelatin methacryloyl/ scleral extracellular matrix (GelMA/dSECM) hydrogel. They were developed via low-temperature extrusion-based 3D printing. The dPS layer provided stable mechanical support with high tensile strength, while the GelMA/dSECM hydrogel exhibited a porous microstructure. Bioactive components released from the bilayered material enhanced human scleral fibroblast (HSF) proliferation, migration, and collagen I expression. Bioinformatic analysis revealed that dSECM core proteins were enriched in extracellular matrix organization and angiogenesis-related pathways. In a form-deprived myopia (FDM) guinea pig model, the bilayered material controlled axial elongation and vitreous chamber depth increase. It promoted scleral thickening and achieved close apposition with host tissue in 4 weeks. This work presents a “mechanical support + regenerative” synergistic system, offering a potential strategy for effective PM management.