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An arsenic biosorbent comprising neem leaves (NL) and MnFe2O4 particles was developed and its removal potential was investigated. Physicochemical analysis of the NL/MnFe2O4 composite (MNL) was performed for the Brunauer, Emmett and Teller surface area, Fourier transform infrared spectra (FT-IR), and scanning electron microscopy-Energy-dispersive X-ray (EDX). The following parameters were optimized: pH, biosorbent dose, contact time, temperature, and initial arsenic concentration. The optimum pH values achieved for biosorption of As(III) and As(V) were 7.0 and 4.0, respectively, when the equilibrium time was 110 minutes for both. MNL was found to be efficient with 85.217% and 88.154% biosorption efficiency at a concentration of 50 mg/L of As(III) or As(V) solution, respectively. This was also proved by the FT-IR study of arsenic-loaded biosorbent. For establishing the best suitable correlation for the equilibrium curves exploiting the procedure of the nonlinear regression for curve fitting analysis, isotherm studies were conducted for As(III) and As(V) using 30 isotherm models. The pattern of biosorption fitted well with Brouers-Sotolongo isotherm model for As(III) and Langmuir-Freundlich as well as Sips isotherm models for As(V). Dubinin-Radushkevich (D-R) isotherm studies specified that ion exchange might play a significant role. The influence of various co-existing ions at different concentrations was examined. Desorption study was performed using various concentrations of NaOH solution.