The raw cladode ofOpuntia ficus indica(OFI) was evaluated as a sustainable biosorbent for the removal of heavy metals (Ni, Pb, Cu, and Cd) from aqueous solutions. The functional groups of OFI were identified by employing DRIFT-FTIR and CP-MAS-NMR techniques before and after contact with the ions in an aqueous media, showing a rearrangement of the biomass structure due to the complexation between the metal and the functional groups. The adsorption process was studied in both single- and multi-component systems under batch conditions at different pHs (4.0, 5.0, and 6.0), different metal concentrations, and different biomass amounts. The results show that the raw OFI had a removal capacity at room temperature of over 80% for all metals studied after only 30 min of contact time, indicating a rapid adsorption process. Biosorption kinetics were successfully fitted by the pseudo-second-order equation, while Freundlich correctly modelled the biosorption data at equilibrium. The results of this work highlight the potential use of the untreated cladode of OFI as an economical and environmentally friendly biosorbent for the removal of heavy metals from the contaminated aqueous solution.