In this paper, a series of self-healing waterborne polyurethane/polyacrylate composites (SWPUA) with different disulfide content on the main chain were synthesized. The SWPUAs were synthesized from isophorone diisocyanate, dimethylolpropionic acid, polyether diol and bis(2-hydroxyethyl) disulfide (HEDS). The structure of the products was characterized by IR and Raman spectra. The effects of different content of HEDS on dispersion stability, mechanical property and self-healing properties (including tensile strength and breaking elongation) of SWPUAs were studied. The results showed that all the prepared SWPUAs have excellent dispersion stability, thermal stability, self-healing efficiency and certain hydrophobic capacity. Thereinto, SWPUA-1 and SWPUA-2 products with HEDS content of 0.0025 mol and 0.0050 mol have the best repair efficiency. They can recover 101.03% and 102.18%, respectively, after 3 h of repair at 75 C. In addition, SWPUA-1 has the highest repeatedly repair efficiency of 91% for tensile strength but 75% for breaking elongation because of the influence of physical entanglement and chain link.