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This study introduces a novel chemically modified silk\u2010based biomaterial to modulate key signaling pathways involved in OA and cartilage repair. The designed biomaterial concurrently inhibits the bone morphogenetic protein (BMP) signaling, aberrantly activated during OA, and inherently facilitates Wnt\/\u03b2\u2010catenin signaling, a crucial factor for chondrogenesis and cartilage homeostasis. The dual modulation was achieved by covalently conjugating the potent BMP inhibitor LDN\u2010193189 to the Silk Fibroin\u2013Gelatin (SF\u2010G) bioink. The chemically decorated SF\u2010G construct served as a biomimetic delivery platform and a mechanically robust support, ideally suited for regenerating load\u2010bearing articular cartilage. The functionalized material was implanted into a critical\u2010sized cartilage defect in the rat femoral trochlear groove, which had been previously subjected to OA by anterior cruciate ligament transection. 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