Intensifying urban stormwater runoff and pollution caused by urbanization and climate change threatens property and lives in cities around the world. Low-impact development (LID) is an effective approach to improve urban flood resistance, but there is a lack of quantitative evaluation criteria to determine the best scenario in the newly built and built-up urban areas. In this study, based on the Fuzzy Comprehensive Evaluation method (FCE), a multi-index evaluation system is established to quantify the LID performance for the environment, technology, economy, and society. For overcoming subjective arbitrariness, the Criteria Importance Though Intercriteria Correlation (CRITIC) and Analytical Hierarchy Process (AHP) methods are used to evaluate the weight of each evaluation index. The proposed method is demonstrated for the Xi’an City, China. Results show that the integrated configuration of green roof, infiltration pavement and grass swale has the best comprehensive efficiency under the proposed method. More specifically, the allocation of different LID combinations in the newly built area can effectively manage the flooding in this area. However, the comprehensive efficiency of increasing the diameter of the storm sewer is optimal in the built-up area. The increased pipe diameter can discharge more rainwater through the urban storm sewer and mitigate overflow. A multi-index evaluation framework beyond the traditional subjective evaluation standard is established, which can quantitatively evaluate the effectiveness of LID facilities. The proposed quantification evaluation method can provide an efficient recommendation for sponge city construction and evaluation.