To fulfil the demands of high-power plant growth lamps, cation co-doping is an effective way to tune the photoluminescence properties of manganese (& x2163;)-activated aluminate phosphors. Therefore, we managed to synthesize a series of cations co-doped CaYAlO4:xMn(4+), mSr(2+), M+ (M+ = Li+, Na+, and K+) (CYAO:Mn, Sr, M) far-red-emitting phosphors. The excitation spectrum of these phosphors contained two excitation bands, and the opposite effects of these two bands on the luminescence intensity have been observed with the increase of Mn4+ concentration. By adding 0.1 mol Sr2+ ions to replace Ca2+ site, the emission intensity and thermal stability of CYAO:Mn phosphors can be enhanced. Furthermore, the luminescence properties of CSYAO:Mn can be further improved by co-doping monovalent alkali metal ions to serve as charge compensators, the increased number of Mn4+ luminescence centers. Moreover, 0.6 mol% Na+ can increase the initial emission intensity of the phosphors by 117% as the best ratio. The characteristic emission spectrum of the phosphors CYAO:Mn,Sr,M correspond to the phytochrome P-FR of plants. These experiments and characterization results have certified that these phosphors have a potential application in indoor plants cultivation.