A new bio-based bilateral hydrogel containing carboxymethyl cellulose (CMC) and polyacrylamide (PAM) was prepared for the wastewater remediation. The obtained CMC/PAM composite hydrogel reveals a strong single-ion affinity for copper (Cu II ), lead (Pb II ) and cadmium (Cd II ) ions, as well as multi-ion absorbability with its equilibrium data following the Langmuir adsorption model and its adsorption process abiding by a pseudo-second-order kinetics. To demonstrate its recycled use for the metal ions, the adsorbed Cu II ions in the hydrogel were reduced in situ to form homogeneously dispersed Cu nanoparticles (NPs), leading to the Cu NPs-loaded CMC/PAM hydrogel. Reduction of 4-nitrophenol to 4-aminophenol with high efficiency was successfully achieved by this Cu NPs-loaded CMC/PAM hydrogel, verifying the hydrogel’s dual functionalities towards the wastewater treatment and catalytic application.