Copper (Cu2+) contamination of water resources presents a continuing risk to ecosystems and human health. Low-cost adsorbents derived from renewable biomass offer a sustainable route to their removal. In this work, cellulose was extracted and converted to nanocellulose. Nanocellulose (42.281 ± 16.111 nm) was produced via optimised phosphoric acid hydrolysis with an acid concentration of 68%. The nanocellulose was crosslinked with the metal-organic framework (MOF). Attenuated Total Reflectance Fourier-transform infrared spectroscopy (ATR-FTIR), X-ray diffraction spectroscopy (XRD), Nuclear magnetic resonance spectroscopy (NMR), and morphological analysis were done using Scanning electron microscopy (SEM), and zeta potential measurements confirmed successful synthesis. FTIR analysis verified the presence of characteristic functional groups associated with the nanocellulose and MOF. XRD analysis revealed the retention of the crystalline structure of nanocellulose following hydrolysis and the successful incorporation of MOF within the composite matrix. NMR confirmed retention of the nanocellulose backbone and successful incorporation of MOF. A four-factor Box-Behnken design of 27 runs was used to evaluate the effects of solution pH, adsorbent dose, initial Cu2+ concentration, and contact time on the equilibrium adsorption capacity (qe). A full quadratic model described the qe response well (R2 = 0.964), identifying adsorbent dose and initial concentration, together with their interaction, as the controlling factors, while pH and contact time were not significant. Kinetic data collected under the optimised conditions followed the pseudo-second-order model (R2 = 0.9946; qe = 20.36 mg g−1), with intraparticle diffusion analysis revealing a fast external-film stage followed by slower pore