The design and preparation of functionalized composite adsorbent materials are of key importance for wide environmental fields. This study demonstrates a new route to fabricate hybrid nanomaterial by encapsulating Schiff base molecules into sulfonate groups charged polystyrene beads (PS). The prepared composite adsorbent, polystyrene-Schiff base ((PS-SB)) nanocomposites, showed more preferable Cu(II) ion removal capacity in the presence of Mg2+ and Ca2+ co-ions in solutions. Comparatively, the obtained (PS-SB) composites with inner well-dispersed Schiff base molecules and high sorption ability demonstrated much faster breakthrough for Cu(II) ion removal than PS beads, mainly due to the electrostatic forces and coordinating reaction of Schiff base groups with Cu(II) ion. In addition, the used composite adsorbent material could be easily regenerated by HCl-NaCl solution for repeated utilization without obvious capacity loss. Present research work showed that charged functional groups in host nanostructures improved the dispersion and connection of anchored organic molecules, enhancing the removal capacity of targeted metal ions. Suitably designed guest molecules in composite structures are crucial in the preparation of excellent nanocomposites for the removal of toxic metal ions and other charged pollutants from wastewater.