In this study, the synthesis and characterization of grafted cellulose fiber with binary monomers mixture obtained using a KMnO4/citric acid redox initiator were investigated. Acrylonitrile (AN) was graft copolymerized with acrylic acid (AA) and styrene (Sty) at different monomer ratios with evaluating percent graft yield (GY%). Cell-g-P(AN-co-AA) and Cell-g-P(AN-co-Sty) were characterized by SEM, FT-IR, 13C CP MAS NMR, TGA, and XRD. An AN monomer was used as principle-acceptor monomer, and GY% increases with AN ratio up to 60% of total monomers mixture volume. The adsorption behaviors of Cell-g-P(AN-co-AA) and Cell-g-P(AN-co-Sty) were studied for the adsorption of Ni(II) and Cu(II) metal ions from aqueous solution. Optimal adsorption conditions were determined, including 8 h contact time, temperature of 30 °C, and pH 5.5. Cell-g-P(AN-co-AA) showed maximum adsorption capacity of 435.07 mg/g and 375.48 mg/g for Ni(II) and Cu(II), respectively, whereas Cell-g-P(AN-co-Sty) showed a maximum adsorption capacity of 379.2 mg/g and 349.68 mg/g for Ni(II) and Cu(II), respectively. Additionally, adsorption equilibrium isotherms were studied, and the results were consistent with the Langmuir model. The Langmuir model’s high determinant coefficient (R2) predicted monolayer sorption of metal ions. Consequently, Cell-g-P(AN-co-AA) and Cell-g-P(AN-co-Sty) prepared by a KMnO4/citric acid initiator were found to be efficient adsorbents for heavy metals from wastewater as an affordable and adequate alternative.