Recently, an increase in impervious area induced by the process of urbanization has significantly affected the quantity and quality of urban surface runoff. Among the pollutants of the storm flow, total suspended solids (TSS) are an extremely important cause of water quality deterioration. This paper aims to use the integrated nondominated sorting genetic algorithm (NSGA II)–Storm Water Management Model (SWMM) method to find optimal Low-Impact Development (LID) plans which ensure maximum TSS load reduction and minimum total relative cost. Green roofs, permeable pavements, and tree boxes with fixed parameters and unit costs were considered for seeking optimal planning alternatives in the Cau Bay river basin. The optimization process yielded a cost–effectiveness curve, which relates cost of LID implementation with its corresponding TSS reduction efficiencies. The advantage of the optimization approach was clarified when, with a defined cost of LID implementation, there was a significant difference in TSS reduction efficiencies between the optimal and non-optimal alternatives. The increase in return periods of rainfall patterns not only resulted in a reduction in the TSS removal efficiencies of LID practices at the outfall of the study area, but also spatially changed in terms of the TSS removal efficiencies of the sub-catchments. The return period of the rainfall patterns utilized for LID design should not exceed 2 years. The simulation–multi-optimization approach facilitates integration of LID practice plans into the urban infrastructure master plans in Vietnam.