The capability of modified spent grain (MSG) to adsorb silver (I) [Ag(I)] from aqueous solution was investigated and compared with raw spent grain (RSG) regarding their adsorption isotherms, kinetics, and thermodynamics. The monolayer adsorption capacity was 30.28 mg/g for RSG and 158.23 mg/g for MSG according to the Langmuir isotherm. The Ag(I) adsorption on MSG was approximately 4 times higher than that on RSG. The pseudo-second-order kinetic model provided the best description of Ag(I) adsorption on the two adsorbents. The calculated activation energy (Ea) implies that the adsorption of Ag(I) on RSG is a physical adsorption and on MSG is of a chemical nature. Thermodynamic results suggest that the adsorption of Ag(I) is an exothermic process for RSG and an endothermic process for MSG, whereas both adsorption processes are spontaneous in nature.