Environmental pollution with organic dyes is increasing due to the discharge of industrial wastewater. Therefore, introducing an efficient adsorbent for removing organic dyes is of great value. For this purpose, a novel reusable nanocomposite hydrogel (NCH) was synthesized with high adsorption properties. This was achieved by in situ formation of ZnO nanoparticles within the κ-carrageenan/talc-g-poly (acrylic acid) hydrogel network. The resulting nanocomposite hydrogel was then applied as an effective adsorbent for removing cationic dyes from wastewater. The NCH was extensively characterized using techniques such as X-ray diffraction (XRD), Fourier transform infrared (FT-IR) spectroscopy, thermogravimetric analysis (TGA), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), Transmission electron microscopy (TEM), and Brunauer–Emmett–Teller (BET) analysis. The effect of pH, contact time, temperature, and dye concentration on adsorption efficiency were evaluated. The removal efficiency of crystal violet (CV) was found to be more than 98% at a concentration of 10 mg/L and pH = 6. Under optimum conditions, the maximum adsorption capacity of the NCH for CV was 350 mg/g. The adsorption isotherm follows the Temkin model. The kinetic studies demonstrated that dye adsorption follows the pseudo-second-order model. The adsorption mechanism involves strong electrostatic interactions between the anionic carboxylate groups present in the NCH and the cationic groups of the CV molecule. Additionally, the increased surface area is provided by the incorporation of ZnO nanoparticles. The thermodynamics of adsorption indicated that the adsorption is spontaneous and exothermic in nature. The reusability study indicated that about 93% of initial adsorption capacity was retained after 10 cycles. Therefore, these environmentally friendly nanocomposite hydrogels exhibit outstanding performance in the treatment of dye-contaminated wastewater.