Soil washing is an important method for the remediation of contaminated soil. This research presents the optimization of soil washing conditions in the remediation of Zn-contaminated soils with water-soluble chitosan (WSCS). Response surface methodology (RSM) was used to optimized the washing conditions after single factor experiments. The central composite design (CCD) with three factors and five levels was applied to the optimization of the removal efficiency of Zn from soils, and WSCS concentration, pH value, and washing time were evaluated variables in the washing process. Results indicated that the pH value (p < 0.0001) was the most significant factor which mainly affected the distribution and content of metal species in aqueous solution, ion exchange and adsorption/desorption behavior of metals, solubility of chelating agent, as well as readsorption of metal complexes. The optimal conditions for the Zn removal from soils were WSCS concentration of 1.5%, pH of 3.3, and washing time of 72 min. The removal efficiency could reach 65.4% under the optimized conditions, which was close to the predicted value of 68.3% by the response surface method. Therefore, it could be found that the response surface methodology was an effective method to determine the optimal conditions for the removal of metals from contaminated soils by soil washing.