Environmental contamination with pesticides occurs at a global scale as a result of prolonged usage and, therefore, their removal by low-cost and environmentally friendly systems is actively demanded. In this context, our study was directed to investigate the feasibility of using some self-assembled hydrogels, comprising chitosan (CS) and carboxymethylcellulose (CMC) or dialdehyde (DA)-CMC, for the removal of four complex fungicide formulations, namely Melody Compact (MC), Dithane (Dt), Curzate Manox (CM), and Cabrio®Top (CT). Porous CS/CMC and CS/DA-CMC hydrogels were prepared as discs by combining the semi-dissolution acidification sol-gel transition method with a freeze-drying approach. The obtained CS/CMC and CS/DA-CMC hydrogels were characterized by gel fraction yield, FTIR, SEM, swelling kinetics, and uniaxial compression tests. The batch-sorption studies indicated that the fungicides' removal efficiency (RE%) by the CS/CMC hydrogels was increased significantly with increasing sorbent doses reaching 94%, 93%, 66% and 48% for MC, Dt, CM and CT, respectively, at 0.2 g sorbent dose. The RE values were higher for the hydrogels prepared using DA-CMC than for those prepared using non-oxidized CMC when initial fungicide concentrations of 300 mg/L or 400 mg/L were used. Our results indicated that CS/DA-CMC hydrogels could be promising biosorbents for mitigating pesticide contamination of aqueous environments.