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The purpose of this paper is to provide new ideas and methods for the sustainable use of groundwater in areas with serious groundwater overexploitation and serious groundwater pollution. Geographic information systems (GIS) were combined with machine learning algorithms, water resources optimization technology, and groundwater numerical simulation to optimize the regulation of the groundwater table and quality beneath the Daxing District in the southern plain of Beijing. By collecting local consumption and supply data and observations of the groundwater table and quality in the connected aquifer beneath Daxing for the years 2006–2020, the corresponding water demands and groundwater impact were extrapolated for the years 2021–2025 based on the basis of the existing development model. Through the combination of GIS and machine learning algorithms, the NO3-N concentration of local groundwater monitoring points in wet years, normal years, and dry years were predicted. With respect to NO3-N pollution, three new groundwater exploitation regimes were devised, which we numbered 1 to 3. The optimal allocation of water resources was then calculated for wet year, typical year, and dry year scenarios for the year 2025. By comparing the water shortage, groundwater utilization rate, and NO3-N pollution under the new groundwater exploitation regimes, the optimal groundwater exploitation mode for the three different types of hydrological year was determined. The results indicate that NO3-N pollution was greatly reduced after the adoption of the optimal regimes and that the groundwater table demonstrated rapid recovery. These results can be of great help in realizing the management, supervision, and regulation of groundwater by combining GIS with machine learning algorithms. [ABSTRACT FROM AUTHOR]