Sludge drying is a necessary step for sludge disposal. In this study, sludge was collected from two wastewater treatment plants, and dried at different temperatures in the laboratory. The emission of odor and total volatile organic compounds (TVOCs) during the sludge drying process were determined by an online odor monitoring system. The volatile organic compounds (VOCs) in off-gas were analyzed by gas chromatography–mass spectrometry. Results showed that sludge with 30% moisture content could be obtained in 51 minutes under drying temperature 100 °C but only within 27 minutes under 150 °C. Concentration of odor, TVOCs, sulfur-containing compounds (SCCs), and amines were changed with drying temperature and sludge sources. The maximum concentration of odor, TVOCs, SCCs, and amines were 503.13 ppm, 3.01 ppm, 8.15 ppm, and 11.27 ppm, respectively, at drying temperature 100 °C. These values reached 1,250.79, 8.10, 53.51, and 37.80 ppm when sludge dried at 150 °C. Odor concentration had a close relationship with emission of SCCs, amines, and TVOCs. The main VOCs released were benzene series and organic acid. Potential migration of substances in sludge was examined via analysis of off-gas and condensate, aiming to provide scientific data for effective sludge treatment and off-gas control.