Although smart windows have received wide attention as energy-saving devices, conventional metal-to-insulator materials such as VO2 hinder their commercial usage because of their high transition temperature and low solar energy modulation. Further development can be achieved by finding a new material system that can effectively overcome these limitations. In this study, first-principles density functional theory calculations are used to investigate the possibility of exploiting a spin-polarized band gap material for smart window applications. Halide cuprite perovskites (A2CuX4) were chosen because they have a spin-polarized band gap that can be tuned by element selection at sites A and X. Our study shows that the optical transmittance of the insulating phase is increased by a violation of the selection rule. The spin-polarized band gap is closely related to the metal-to-insulator transition temperature and can be modulated by chemical engineering, strain engineering, or both. Therefore, A2CuX4 is a promising candidate for smart windows.