Stone powder (SP) produced from masonry mills has been treated as a specific waste and rarely used for environmental purposes. In this study, we tested its potential as an adsorbent to remove arsenic (As) and lead (Pb) from water. The single-solute sorption isotherms for As(V) and Pb(II) onto SP and chitosan-coated SP (CSP) were investigated. Several sorption models, such as the Langmuir, Freundlich, and Dubinin−Radushkevich (DR) models, were used to analyze the adsorption features. The results demonstrated that As and Pb were successfully adsorbed onto SP and CSP, indicating that SP and CSP had potential as adsorbents of As and Pb. The maximum adsorption capacities of SP and CSP for Pb were 22.8 and 54.5 times higher than those for As, respectively. Chitosan coating increased the adsorption potential in Pb adsorption by 5% but decreased it in As adsorption. The adsorption potential also depended on the pH and temperature. The adsorption amount of As increased with pH but that of Pb decreased as pH increased. In addition, the ln b in the Langmuir model increased with 1/T (K), indicating that the adsorption of As and Pb occurred exothermically and spontaneously.