Novel hydrogels composed of thermo-responsive poly(N-isopropylacrylamide) (PNIPAM) and redox-responsive poly(ferrocenylsilane) (PFS) macromolecules were formed by photopolymerization. PFS chains bearing acrylate side groups were copolymerized with NIPAM and N,N’-methylenebisacrylamide in tetrahydrofuran in a predetermined ratio under ultraviolet light-emitting diode (UV-LED) irradiation at a wavelength of 365 nm, in the presence of a photoinitiator. Crosslinking occurred smoothly, providing homogeneous hydrogels. The equilibrium swelling ratio, rheology and morphology of these hybrid PNIPAM-PFS-based hydrogels were investigated. In-situ fabrication of silver nanoparticles inside the hydrogel network via reduction of silver nitrate by the PFS chains led to hydrogel composites. These composites showed strong antimicrobial activity while maintaining a high biocompatibility with cells.