Efficient wastewater treatment, particularly the removal of heavy metal ions, remains a challenging priority in environmental remediation. This study introduces a novel sandwich-structured nanocomposite, RGO-CuS-PPy, composed of reduced graphene oxide (RGO), copper sulfide (CuS), and polypyrrole (PPy), synthesized via a straightforward hydrothermal method. The unique combination of RGO, CuS, and PPy offers enhanced adsorption capacity for Ni(II) ions due to RGO’s high surface area and CuS’s active binding sites, supported by PPy’s structural stability contributions. This study is among the first to explore this specific nanocomposite architecture for Ni(II) removal, achieving an adsorption capacity of 166.67 mg/g and a high removal efficiency of 94.9% within 210 min for 55 mg/L of Ni(II) concentration at pH 6 and adsorbent dose of 3 mg/15 mL. The kinetic analysis shows the best fitted time-dependent experimental data with the pseudo-second-order model, indicating chemisorption. Isotherm studies confirmed the Langmuir model as the best fit, yielding a high monolayer adsorption capacity of 166.67 mg/g. Thermodynamic analysis shows the adsorption process was endothermic (ΔH° = 80.23 kJ/mol) and spontaneous (ΔG° ranging from −6.985 to −14.399 kJ/mol). Additionally, reusability tests using 0.1 M HCl for desorption demonstrated good reusability, emphasizing the RGO-CuS-PPy nanocomposite’s potential as a sustainable adsorbent for Ni(II) removal in wastewater treatment applications.