An increase in the production of cationic dyes is expected over the next decade, which will have an impact on health and the environment. This work reports an adsorbent hydrogel composed of poly(acrylic acid) [poly(AA)] and Fe₃O₄ particles, prepared by radical polymerization and in situ co-precipitation of Fe³⁺ and Fe²⁺. This Fe₃O₄/poly(AA) composite hydrogel was used to evaluate its potential for removing the cationic dyes methylene blue (MB) and crystal violet (CV) from aqueous solutions. Instrumental characterization of the hydrogel was performed by FTIR, XRD, TGA, VSM, and physicochemical analysis (swelling and response to changes in pH). The results show that the incorporation of Fe₃O₄ particles improves the adsorption capacity of MB and CV dyes to a maximum adsorption of 571 and 321 mg/g, respectively, under the best conditions (pH 6.8, dose 1 g/L, time 24 h). The adsorption data best fit the pseudo-first order (PFO) kinetic model and the Freundlich isothermal model, indicating mass transfer via internal and/or external diffusion and active sites with different adsorption potentials. Moreover, the thermodynamic analysis confirmed that the adsorption process was spontaneous and exothermic, with physisorption as the dominant mechanism. In addition, the Fe₃O₄/poly(AA) hydrogel is capable of removing 95% of the dyes after ten consecutive adsorption–desorption cycles, demonstrating the potential of hydrogels loaded with Fe₃O₄ particles for the treatment of wastewater contaminated with dyes.