The difficulty of residual sludge dehydration is the major problem in sewage treatment. The reduction of moisture content in sludge can reduce the sludge volume significantly and is conducive to the subsequent disposal of sludge. As an organic polymer flocculant, chitosan (CTS) is widely used in water and waste water treatment. In this study, CTS was used in sludge treatment to improve the sedimentation and dehydration properties of sludge. When treated with CTS, the moisture content of sludge cake decreased from 85.9% to 83.0%, the SV30 decreased to about 1/2, and the sludge volume reduced to 82.9%. Further analysis showed that the zeta potential (ζ-potential) of the sludge changed from negative value to positive value, and the D50 of the sludge was larger than that of the raw sludge. In addition, when the moisture content of the sludge cake was reduced to the lowest, the concentration of extracellular polymeric substances (EPS) and SCOD was the largest and the |ζ| decreased to the lowest. CTS improved the dehydration and sedimentation performance of sludge mainly by factors of electrical neutralization, adsorption bridging and dissolution of EPS.