Heavy metals (HMs) in water are highly poisonous and carcinogenic agents for human health. To alleviate the toxic impacts of HMs, green remediation technologies are the need of the hour. In this regard, different nanosorbents (CMCG@ORP, ORAC, NiO/NPs, and NiO@ORAC/NCs) were synthesized in the present study, and the percentage removal of heavy metals [chromium(VI) and cadmium(II) ions] was evaluated. The nanosorbents were characterized by using FTIR, SEM, UV–Vis spectroscopy, and XRD. UV–Vis spectroscopy confirmed the synthesis of nanosorbents such as NiO/NPs and NiO@ORAC/NCs at 330.5 nm and 352.55 nm, respectively. The characterization studies show that the surface of synthesized nano-sorbents was highly coarse, uneven, and abrasive. XRD pattern deduced that the sample was of single phase, and no other impurity was detected except the face-centered cubic-phase peak of NiO. The maximum adsorption of Cd (91%) and Cr (92%) was found at initial concentrations of 100 and 60 ppm respectively at contact time = 180 min, temperature 25 °C, and with an adsorbent dose of 0.5 g. Isothermal, kinetic, and thermodynamic studies were also performed to evaluate the adsorption mechanisms and feasibility of the process. Adsorption mostly followed Freundlich isotherm which indicates the multilayer adsorption phenomenon and the negative value of Gibb’s free energy showed the spontaneous nature and feasibility of the adsorption reaction. Surface complexation, ion exchange, surface precipitation, and the phenomenon of physical adsorption occurred on the sorbent surface which led to the attachment of Cd and Cr to the tested nanosorbents. In conclusion, NiO@ORAC/NCs were the most effective in the alleviation of Cd(II) and Cr(VI) ions in contaminated water.