In this study, first, the ter-polymerization reaction between vinyl pivalate (VP), maleic anhydride (MA), and N-tert-butylacrylamide (NTBA) was done in inert atmosphere (N2). FT-IR and 1HNMR spectroscopy was applied to study the chemical composition of the obtained ter-polymers. MA content of the ter-polymers was determined by following the chemical titration method. Second, novel chitosan/ter-(vinyl-pivalate-maleic-anhydride-N-tert-butylacrylamide) microcapsules were synthesized. In microcapsule production, chitosan polymer served as a matrix for acrylamide ter-polymers with four different molar ratios. The microcapsules were characterized by FT-IR and SEM analyses. Cu(II) sorption efficiency of the microcapsules were tested at different pH levels, temperature, sorbent dosage, and metal ion concentration. Comparison with blank chitosan microbeads revealed that incorporation of acrylamide ter-polymers into the cross-linked chitosan matrix increased the metal sorption. Sorption capacities of the sorbents were recorded; blank chitosan microbeads: 67.03 mg g−1, and chitosan/acrylamide ter-polymer microcapsules: in range of 75.39–98.64 mg g−1. The findings demonstrated chitosan/acrylamide ter-polymer microcapsules can be utilized in sorption of Cu(II) ions in water treatment.