AbstractWith a small amount of isocyanate‐terminated polysulfide (NCO‐PSF‐NCO) as additive, the commercial polysulfide‐based sealant had significant improvement in mechanical properties. The test results showed that 5% of NCO‐PSF‐NCO could help to rise 50% in the tensile strength and 27% in the ultimate elongation of the polysulfide sealant. The adhesive strength to substrates such as steel, epoxy‐coated or polyurethane‐coated surface also increased significantly. Dynamic mechanical thermal analysis and differential scanning calorimetry analysis revealed that formed polysulfide polythio‐urethane‐urea (polysulfide‐urea) contributed to a slight increase in the Tg of the polysulfide sealant. It might be due to the domains of polysulfide‐urea, which had effects of physical crosslinking and chain‐extending on the polysulfide sealant. However, the introduction of polysulfide‐urea structures had no appreciable influence on oil resistance of the polysulfide sealant. © 2007 Wiley Periodicals, Inc. J Appl Polym Sci, 2007