In our previous work, three different weight ratios of chitosan/PVA (1:3, 1:1, and 3:1) were blended and then cross-linked with trimellitic anhydride isothiocyanate (TAI) at a concentration depending on their chitosan content, obtaining three hydrogels symbolized by H, H, and H. Pure chitosan was cross-linked with TAI, producing a hydrogel symbolized by H. Further, three H-based silver nanoparticles composites (H/AgNPs1%, H/AgNPs3%, and H/AgNPs5%) were also synthesized. They were investigated, for the first time in this study, as adsorbents for Congo Red (CR) and Crystal Violet (CV) dyes. The removal efficiency of CR dye increased with increasing H content in the hydrogels, and with increasing AgNP content in the composites, reaching 99.91% for H/AgNPs5%. For CV dye, the removal efficiency increased with the increase in the PVA content. Furthermore, the removal efficiency of CV dye increased with an increasing AgNP content, reaching 94.7% for H/AgNPs5%. The adsorption capacity increased with the increase in both the initial dye concentration and temperature, while with an increasing pH it increased in the case of CV dye and decreased in the case of CR dye. The adsorption of CV dye demonstrated that the Freundlich isotherm model is better suited for the experimental results. Moreover, the results were best fitted with pseudo-second-order kinetic model.