The basin economy is essential in China’s high-quality development, which brings prodigious economic and social benefits. However, high industrialization and urbanization led to a significant escalation in water pollution within basins. The achievement of synergistic control of water environment pollution at the basin scale has emerged as a primary goal for governmental departments in developing environmental policies. This study constructs a “four-in-one” basin’s water environment regulation system comprising four categories: total, quality, project, and governance. Further, the spatial spillover effects of water environment pollution control in 27 Chinese provincial-level administrative regions spanning key river basins were analyzed. This study aims to provide evidence from China on the transfer of water pollution in basins worldwide. The results indicate the following conclusions: (1) A consistent upward trend in the environmental regulations and water environment pollution indexes across all provinces in the basin. Compared to 2006, in 2018, the mean value of the basin environmental regulation index was 0.21, which is an increase of 23.5%, and the mean value of the water environmental pollution index was 0.83, which is an increase of 29.7%. (2) Whether in the basin’s upper, middle, or lower reaches, the relationship between environmental regulations and water pollution follows a “U”-shaped pattern, with thresholds of 0.318, 0.331, and 0.390, respectively. (3) Under the neighbor weight matrix and water flow distance weight matrix, the impact coefficient of the water environment pollution index on the surrounding areas is significantly positive, implying that the implementation of local environmental policies will radiate to the neighboring areas in the short term and bring positive governance effects. (4) Regarding the time-lag effect, it is observed that the lag term associated with the water environment pollution index exhibits a statistically significant positive relationship. This finding suggests that the pollution of the water environment within the basin follows a cumulative and continuous pattern. (5) It is noted that long-term environmental regulation measures do not contribute favorably to the amelioration of water pollution in the neighboring regions. This implies the presence of a characteristic neighboring avoidance effect.