Dye contamination is a serious environmental issue, particularly affecting water bodies, driving efforts to synthesize adsorbent materials with high dye-removal capacities. In this context, eco-friendly and cost-effective materials derived from bioresidues are being explored to recycle and valorize waste. This study investigates the synthesis, characterization, and application of a biohydrogel made from unripe plantain peel (PP), modified with carboxymethyl groups and crosslinked using varying concentrations of citric acid (CA), an eco-friendly and economical organic acid. The materials were characterized by ATR-FTIR, TGA, and SEM, confirming the successful synthesis of hydrogels, which exhibited rough, irregular surfaces with micropores. Additionally, the materials were analyzed for their pH point of zero charge, swelling capacity, and methylene blue (MB) dye removal efficiency. The results indicate that the biohydrogel formed with 1% CA exhibited the most favorable characteristics for MB removal. Kinetic studies revealed that the adsorption mechanism is pH-dependent, with equilibrium being reached in 720 min. The Freundlich isotherm model provided the best fit for the adsorption data, suggesting a heterogeneous surface and a multilayer adsorption process, with a maximum retention capacity of 600.8 ± 2.1 mg/g at pH 4. These findings contribute to the development of cost-effective and efficient materials for dye removal, particularly from water bodies.