Engineered cementitious composites (ECC) have higher ultimate tensile strains than normal concrete. The mechanical properties of ECC strongly depend on raw materials and the mix proportions. The uniform design test method and alternating conditional expectation, which is a nonparametric regression analysis method, were used to design the ECC mix proportion. According to the regression analysis, the optimized W/B, S/B, and F/B ranges could be obtained as 0.35–0.42, 0.25–0.3, and 0.02, respectively. The tested proportions for validation were randomly adopted within the range of W/B, S/B, and F/B. The uniaxial compression, tension, and four-point bending tests were conducted to verify the material behaviour of the designed ECC. Results showed that all the specimens had large ultimate tensile strains and high fracture energy capacities, and strain hardening was also observed. The fibers were found to be uniformly distributed in the specimens by using a scanning electron microscope. This paper may provide theoretical and practical guidance for the ECC and other cement-based material mix proportion design.