Polypropylene fibers are added to concrete to improve the toughness of the material. Manufactured sand and fly ash with high content are used to reduce the impact on the environment and cost. The response surface method (RSM) was used to design the test and study the mechanical and bending properties of polypropylene-fiber-reinforced high-performance concrete (PPFHPC). Three process variables, including the content of polypropylene fiber (1%, 1.5%, and 2%), content of fly ash (45%, 60%, and 75%), and water-binder (W/B) ratio (0.27, 0.3, and 0.33), were considered as factors. The compressive strength, flexural strength, flexural-compressive ratio, splitting tensile strength, and first-crack strength and bending strength of thin plate were evaluated. The prediction model established by the RSM showed the correlation and predictability between the response and the factors, and the corresponding relationship equation between the factors and the response was obtained. Results of multiobjective optimization indicated that the optimal three factors (content of PPF, FA, and W/B) were 2%, 62%, and 0.27. The established model can be used to predict the basic mechanical properties and bending properties of materials. This test laid a theoretical foundation for the development of PPFHPC materials.