This study explores the development of a photo-/thermo-responsive bioink for improved printability in extrusion-based bioprinting. The bioink, composed of silk fibroin (SF) and iota-carrageenan (CG), was designed to balance rheological properties and biochemical functionality. Photo-crosslinking of SF and the rapid sol-gel transition of CG enhanced printability and structural integrity of 3D constructs. The resulting bioink exhibited a Young’s modulus of approximately 250 kPa, suitable for keratinocyte and myoblast cell culture. High cell adhesion and viability (up to ~98%) were observed, making the bioink promising for skin and muscle tissue applications. The study also evaluated the mechanical properties, swelling ratio, contact angle, rheological properties, and biodegradability of the SF/CG bioink, demonstrating its potential for tissue regeneration. The optimized SF/CG bioink, particularly SF91CG9, showed superior printability, shape fidelity, and biocompatibility, making it a promising candidate for extrusion-based bioprinting in various biomedical applications.This study explores the development of a photo-/thermo-responsive bioink for improved printability in extrusion-based bioprinting. The bioink, composed of silk fibroin (SF) and iota-carrageenan (CG), was designed to balance rheological properties and biochemical functionality. Photo-crosslinking of SF and the rapid sol-gel transition of CG enhanced printability and structural integrity of 3D constructs. The resulting bioink exhibited a Young’s modulus of approximately 250 kPa, suitable for keratinocyte and myoblast cell culture. High cell adhesion and viability (up to ~98%) were observed, making the bioink promising for skin and muscle tissue applications. The study also evaluated the mechanical properties, swelling ratio, contact angle, rheological properties, and biodegradability of the SF/CG bioink, demonstrating its potential for tissue regeneration. The optimized SF/CG bioink, particularly SF91CG9, showed superior printability, shape fidelity, and biocompatibility, making it a promising candidate for extrusion-based bioprinting in various biomedical applications.