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The full-thickness articular cartilage defect (FTAC) is an abnormally severe grade of articular cartilage (AC) injury. An osteochondral autograft transfer (OAT) is the recommended treatment, but the increasing morbidity rate from osteochondral plug harvesting is a limitation. Thus, the 3D-printed bilayer’s bioactive-biomaterials scaffold is of major interest. Polylactic acid (PLA) and polycaprolactone (PCL) were blended with hydroxyapatite (HA) for the 3D-printed bone layer of the bilayer’s bioactive-biomaterials scaffold (B-BBBS). Meanwhile, the blended PLA/PCL filament was 3D printed and combined with a chitosan (CS)/silk firoin (SF) using a lyophilization technique to fabricate the AC layer of the bilayer’s bioactive-biomaterials scaffold (AC-BBBS). Material characterization and mechanical and biological tests were performed. The fabrication process consists of combining the 3D-printed structure (AC-BBBS and B-BBBS) and a lyophilized porous AC-BBBS. The morphology and printing abilities were investigated, and biological tests were performed. Finite element analysis (FEA) was performed to predict the maximum load that the bilayer’s bioactive-biomaterials scaffold (BBBS) could carry. The presence of HA and CS/SF in the PLA/PCL structure increased cell proliferation. The FEA predicted the load carrying capacity to be up to 663.2 N. All tests indicated that it is possible for BBBS to be used in tissue engineering for AC and bone regeneration in FTAC treatment.