The great spray area of a Super Large-Scale Natural Draft Cooling Tower (SLNDWCT) makes it difficult to achieve an uniform wind field, and non-uniform water spray distributions are adopted in engineering. In this paper, to improve the cooling performance, optimized non-uniform water spray distributions are designed by utilizing network hydraulic calculations and numerical simulations. In the network calculations, the node-formula is applied to figure out the water pressure and flow rate of each spray nozzle, providing more precise data in simulations for the heat and mass transfer. Simulations for operating in summer, Spring/Autumn and winter seasons, which are different in water spray density, have been presented. In the operating in summer, the spray zone is divided into two regions (inner and outer regions), and by adjusting the water spray density and areas of the two regions, an improved water distribution is achieved.