Surplus, low value agricultural by-products can be made into granular activated carbons (GACs) which are used in environmental remediation. This study characterized and evaluated GACs, made from these feedstocks, as effective removers of organics and metals from water. The by-products included soft lignocellulosics such as rice straw, soybean hull, sugarcane bagasse, peanut shell, and harder materials such as pecan and walnut shells. The softer materials were combined with a binder, molasses, to produce briquettes and pellets. The precursors were CO2- or steam-activated, and subsequent treatments included oxidation to enhance metal adsorption. Many of the GACs had acceptable physical GAC attributes, such as durability, for commercial usage. GACs made from pecan and walnut shells adsorbed higher levels of benzene, toluene, methanol, acetonitrile, acetone, and 1,4-dioxane from an aqueous mixture than commercial GACs. Neither CO2 nor steam activation was particularly advantageous in enhancing metal adsorption. Oxidation using O-2-N-2 gas increased metal adsorption while (NH4)S2O8 solution did not In a copper solution, oxidized GACs made from soybean hull had three to four times the Cu(II) adsorption capacity of metal-adsorbing, commercial GACs. Oxidized GACs made from soybean hull, sugarcane bagasse, peanut shell, and rice straw adsorbed from a mixture higher amounts of Pb(II), Cu(II), Ni(II), Cd(II) and Zn(II) than any commercial GACs. Commercial GACs adsorbed only Pb(II), Cu(II) and Cd(II). The GACs made from the agricultural by-products have considerable potential for adsorption of organics and metals of environmental concern.