Single-phase nanomaterials are the most promising materials, owing to their high luminous-efficiency, environmental-friendly and multicolor-luminance features. The crystal structure of Eu3+/Tb3 + co-doped SrLaAlO4 (SLAO) nanopowders were developed by combustion synthesis (CS). The formation of SLAO materials with tetragonal space group 14/mmm (139) was confirmed by Rietveld refinement of X-ray diffraction (XRD) arrangement. Multicolor luminescence has been achieved via tailoring Tb3+/Eu3+ ratio into SLAO matrix, under UV and near-UV irradiation. Moreover, energy-transfer (ET) efficiencies and analogous mechanisms have been discussed deeply. This work opens avenues for scholars to explore such nanomaterials for advanced photonic applications like white-LEDs, solar-cells, lasers, photo-detectors, etc.