Bioremediation of arsenic by medicinal plants had been studied in the present paper. Cascabela thevetia (Kaner) having few anticancer properties and Tinospora cordifolia (Giloy) may adversely affect the health if grown on arsenic contaminated soil. Different initial concentrations of arsenic i.e. 5 ppm, and 2 ppm had been taken at different pH values of 2, 7, and 9 to find the optimum condition of maximum bioremediation using C. thevetia and T. cordifolia. The peaks in HPLC at 227 nm of the plants had shown the changes in peaks before and after treatment. The FTIR peaks also showed changes before and after adsorption. When an initial concentration of 5 ppm As(III) was treated with T. cordifolia at pH 7, the residual concentration was 0.15 ppm. Whereas the residual concentration with 2 ppm initial concentration of As(III) was 0.10 ppm at pH 7. The Maximum percentage removal using C. thevetia treated with the initial concentration of 5 ppm As(III) was 97% at pH 9. No considerable effect of pH had been observed on arsenic remediation. The experimental data best fitted the pseudo-second order reaction.