In this Article, large and uniform Ag nanoparticle-containing hybrid hydrogels were prepared by in situ reduction of Ag ions in cross-linked tapioca dialdehyde starch (DAS)-chitosan hydrogels. In the hybrid hydrogels, chitosan was chosen as a macromolecular cross-linker because of its abundant source and good biocompatibility. The hybrid hydrogel showed good water-swelling properties, which could be controlled by varying the ratio of chitosan to tapioca DAS in the hydrogel. The reductive aldehyde groups in the cross-linked hydrogels could be used to reduce Ag ions to Ag nanoparticles without any additional chemical reductants. Interestingly, by controlling the reduction conditions such as the tapioca DAS concentration, aqueous AgNO3 concentration, reaction time, and aqueous ammonium concentration, Ag nanoparticles with different sizes and morphologies were obtained. Because of their biocompatibility, degradable constituents, mild reaction conditions, and controlled preparation of Ag nanoparticles, these tapioca DAS-chitosan/Ag nanoparticle hybrid hydrogels show promise as functional hydrogels.