Herein, for the first time, natural clinoptilolite-rich zeolite powders modified with a bio-inspired adhesive, polydopamine (PDA), have been systematically studied as an adsorbent for copper cations (Cu(II)) from aqueous solution. Fourier transform infrared (FTIR) spectroscopy, X-ray photoelectron spectroscopy (XPS) and thermogravimetric analysis (TGA) revealed successful grafting of PDA onto the zeolite surface. The effects of pH (2–5.5), PDA treatment time (3–24 h), contact time (0 to 24 h) and initial Cu(II) ion concentrations (1 to 500 mg dm−3) on the adsorption of Cu(II) ions were studied using atomic absorption spectroscopy (AAS) and neutron activation analysis (NAA). The adsorption behavior was fitted to a Langmuir isotherm and shown to follow a pseudo-second-order reaction model. The maximum adsorption capacities of Cu(II) were shown to be 14.93 mg g−1 for pristine natural zeolite and 28.58 mg g−1 for PDA treated zeolite powders. This impressive 91.4% increase in Cu(II) ion adsorption capacity is attributed to the chelating ability of the PDA on the zeolite surface. Furthermore studies of recyclability using NAA showed that over 50% of the adsorbed copper could be removed in mild concentrations (0.01 M or 0.1 M) of either acid or base.