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This study aimed to investigate the biosorption potential of Na2CO3-modified Aloe barbadensis Miller (Aloe vera) leaf (MABL) powder for removal of Ni(II) ions from a synthetic aqueous solution. Effects of various process parameters (pH, equilibrium time, and temperature) were investigated in order to optimize the biosorptive removal. The maximum biosorption capacity of MABL was observed to be 28.986 mg/g at a temperature of 303 K, a biosorbent dose of 0.6 g, a contact time of 90 min, and a pH value of 7. Different kinetic models (the pseudo-first-order, pseudo-second-order, Elovich, and intraparticle diffusion models) were evaluated. The pseudo-second-order kinetic model was found to be the best fitted model in this study, with a coefficient of determination of R2 ? 0.974. Five different isotherm models (the Langmuir, Freundlich, Temkin, Dubinin-Radushkevich, and Brunauer-Emmett-Teller (BET) models) were investigated to identify the best-suited isotherm model for the present system. Based on the minimum chi-square value (x2 ? 0.027) and the maximum coefficient of determination (R2 ? 0.996), the Langmuir isotherm model was found to represent the system well, indicating the possibility of monolayer biosorption. The sticking probability (S*) was found to be 0.41, suggesting a physisorption mechanism for biosorption of Ni(II) on MABL. The biosorbent was characterized using Fourier-transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), zeta potential, and BET surface area, in order to un-derstand its morphological and functional characteristics.