This study investigates the interfacial bond behavior between rebars and polyethylene (PE)-steel hybrid fiber-engineered cementitious composites (HECC). Based on the uniaxial tensile and cube compressive test results of HECC, a predictive model for the ultimate bond strength was established, incorporating a hybrid effect of PE and steel fibers. In addition, 11 sets of pull-out tests were conducted to systematically assess the influence of rebar diameter, matrix compressive strength, relative steel/PE fiber content, and anchorage length on bond performance. Four failure modes were summarized. Based on the measured rebar strain along the bond length, a bond stress position function was derived to characterize the bond stress distribution. Finally, the existing bond-slip constitutive model was modified according to the measured data to establish a constitutive model applicable to rebar and HECC, which was of great significance for the numerical analysis and design of rebar-reinforced HECC structural components.