A cross-linked cellulose-amine polymer composed of nanocrystalline cellulose and 1,4-pheneylnediamine was synthesized, and its application as an adsorbent of metal ions from wastewater was dementated. The nanocrystalline cellulose was generated from an olive industry solid waste. The cross-linked polymer analysis results of FTIR, NMR, TEM, SEM, and XRD were generated. The adsorption efficiency of the cellulose-amine polymer toward Cu(II) and Pb(II) was investigated as a function of adsorbent dose, temperature, pH, and time. The adsorption parameters that lead to an excellent adsorption efficiency were determined. The polymer also showed an excellent extraction efficiency toward 20 metal ions present in a sewage sample. The various functional groups present on polymer surface such as amino, hydroxyl, and aryl played a crucial role on metal adsorption. Thermodynamic analysis results support the high efficiency of the polymer toward the metal ions. Kinetic study results reveal that the adsorption process fits well with the pseudo-second-order model and the adsorption isotherm follows a Langmuir isotherm model.