Silver doped zinc oxide nanoparticles (ZANPs) were synthesized by the gelatin mediated and polymerized sol-gel method, and a calcination temperature of 700 °C was applied for 2 h. X-ray diffraction (XRD), FESEM, TGA, DSC, and EDS were performed to study the structure of the prepared nano-powders. Both cubic silver and hexagonal ZnO diffraction peaks were detected in the XRD patterns. The XRD results, analyzed by the size strain plot (SSP) and Scherrer methods, showed that the crystalline sizes of these nanoparticles increased as the Ag concentration increased. The results were observed via transition electron microscopy (TEM), where the particle size of the prepared samples was increased in the presence of silver. Catechin was chosen as a drug model and was loaded into the hydrogels for release studies. The drug content percentage of catechin in the hydrogels showed a high loading of the drug, and the highest rate was 98.59 ± 2.11%, which was attributed to the Zn0.97Ag0.03O hydrogels. The swelling of the samples and in vitro release studies were performed. The results showed that Zn0.91Ag0.09O showed the highest swelling ratio (68 3.40%) and, consequently, the highest release (84) within 300 min. The higher amount of silver ions in the hydrogel structure causes it to enhance the osmotic pressure of the inner structure and increases the relaxation of the structure chain.