Chitosan-based copolymers (CH-GL1:6, CH-GL1:1, CH-GL1:0.5, and CH-GL1:0.25) were prepared at variable weight ratios of chitosan (CH) to glutaraldehyde (GL). Physiochemical properties of cross-linked copolymers were characterized using FTIR (Fourier Transform Infrared) spectroscopy, PXRD (Powder X-ray Diffraction), CHN analysis, and thermogravimetric analysis (TGA). The swelling behaviour of the polymers along with chitosan was investigated. The sorption properties of copolymers with arsenate oxoanions were investigated at various pH using 10 mM phosphate buffer systems and also in aqueous solution without buffer. The Sips sorption model describes the best fit parameters for adsorption. The relative monolayer sorption capacities Qm (mg/g) of the adsorbents are given in parentheses in the following order: CH-GL1:1(14.4) > CH-GL1:0.5(12.0) > CH-GL1:0.25(10.3) > CH-GL1:6(2.24). In general, the sorption capacities are listed in descending order as follow: un-buffered > buffered (pH 5.0) > buffered (pH 8.5). The removal efficiencies for 20 mg of polymers over a variable concentration range ( 1-200 mg/L) of arsenate in aqueous solution without buffer are as follow: CH-GL-1:1(20-95%), CH-GL1:0.5(14-97%), CH-GL1:0.25(10-98%), CH-GL1:6(2.0-56%), and CH (0.007-3.9%). The sorption properties of the adsorbents were also determined in bicarbonate buffer to evaluate the competitive effect of phosphate buffer on adsorption of arsenate oxoanions. X-ray absorption spectroscopy (XAS) of chitosan and CH-GL1:1 was performed after adsorption at different pH conditions using two buffer systems to evaluate the chemical environment around the arsenate species. In addition, sorptive properties of phenolic adsorbate (i.e. PNP) were estimated with CH-GL copolymers at various pH conditions. The estimated sorptive capacities (Qm; mmol/g) for PNP are in the range 0.07-0.21(mmol/g) while removal efficiencies for PNP are greater at lower pH conditions.