Among the Cu(II) removal methods, adsorption is a favorable technique and has attracted large attention because of its effectiveness and low cost. In quest of seeking for a favorable adsorbent with a high Cu(II) adsorption capacity and excellent reusability, researchers have paid much attention to hydrogels with three-dimensional networks. In this study, a novel hydrogel (P(AMPS-co-VDT) hydrogel) based on free-radical polymerization was synthesized with ionic monomer sodium 2-acrylamido-2-methylpropane sulfate (AMPS-Na +) and 2-vinyl-4, 6-diamino-1, 3, 5-triazine (VDT) and applied for Cu(II) adsorption in aqueous solutions. The hydrogel was characterized for swelling performance, surface morphology, functional groups, thermal gravimetric behavior, and elements. The maximum Cu(II) adsorption capacity (175.75 mg/g) was relatively high compared with other hydrogels. The P(AMPS-co-VDT) hydrogel also was found to have a relatively good Cu(II) desorption and reuse behavior. The adsorption mechanism could be chelation and ion exchange. This work provides a new hydrogel for effective Cu(II) removal in the future.