Herein, we report the preparation, structural and luminescent behaviour of the perovskite LaAlO3:Tb3+ nanophosphors. The low temperature gel-combustion method was employed for the preparation of the present La1−xAlO3:xTb3+ (x = 0.01–0.09) nanomaterials. The crystalline nature and other unit cell parameters were calculated by diffraction pattern and refined data of Rietveld. The present perovskite nanophosphor was found to be cubic crystal having space group Pm3̅m with space number 221. Transmission electron microcopy image has affirmed the smooth morphology, uniform distribution of particles (20–60 nm) with some agglomeration. The analysis of chemical bonding with vibrational characteristics was done by Fourier transform infrared (FTIR) spectroscopy. The information about elemental composition of the selected phosphor was obtained with the help of EDX analysis. In PL spectra recorded at λex= 266 nm, the dominating emission was obtained on 543 nm for 5D4→7F5 in the greenish spectral region. The appropriate color coordinates in the intense green region confirmed the potentiality of LaAlO3:Tb3+ nanophosphors in the display devices and other lighting applications.