The granular activated carbon/MnFe2O4 composite with a mass ratio of 2:1 was synthesized using a simple chemical coprecipitation procedure and used for the removal of As(III) and As(V) from synthetically prepared wastewater. Physicochemical analysis of the composite was carried out through Brunauer, Emmett and Teller surface area and total pore volume, Fourier Transform Infrared Spectroscopy (FT-IR) and Scanning Electron Micrograph and Energy-Dispersive X-Ray Spectroscopy (SEM-EDX). The impact of various adsorption parameters such as the initial pH, adsorbent dose, contact time, temperature and initial arsenic concentration were systematically investigated to evaluate the optimum operating conditions. Nonlinear regression analysis was employed to identify the best-fit isotherm on the basis of three correlation coefficients and three error functions and also to predict the parameters involved in one one-parameter, six two-parameter, nineteen three-parameter, three four-parameter and one five-parameter isotherms. The maximum adsorption capacities estimated using the Langmuir model were 1253mg/g for As(III) and 1314mg/g for As(V) at 30 degrees C temperature and 70min contact time. The results showed that As(III) and As(V) removal was strongly pH-dependent with an optimum pH value of 7.0 and 4.0, respectively. The mean adsorption energy (E) calculated from the D-R model indicated the nature of adsorption being ion exchange type.