The low-carbon city pilot policy is an integral part of China’s efforts to achieve green development. For the purpose of evaluating how well low-carbon city pilot policies work on urban environmental pollution control, this article cites the second batch of pilot cities as an example. With reference to the panel data covering 60 prefecture-level cities, including the second-group pilot cities and some non-pilot cities in the central, western, and eastern regions from 2007 to 2021, a DID model is used to evaluate the policy effect. The research finds that: (1) The implementation of low-carbon city pilot policies contributes effectively to enhancing urban environmental pollution governance performance. (2) In comparison with the eastern and western regions, the policy appears to have a significantly better environmental pollution control effect in the central region. (3) The analysis of the mechanism shows that the pilot policies for low-carbon cities can enhance the urban environmental pollution control effect by raising the ratio of tertiary industry added value and promoting industrial structure optimization and upgrading.