In the prevailing study, single- phased color- tunable La1-x-yEuxTbyAlO3 co- doped nanocrystalline phosphors have been synthesized via the most simplistic and low cost urea- aided solution combustion synthetic route. This was done by adjusting the doping concentration of Eu3+ (x = 0.01, 0.03, 0.05, 0.07 mol) and Tb3+ (y = 0.03 mol) ions in the LaAlO3 host lattice. The X- ray powder diffraction (XRD) and Rietveld refinement analysis confirmed the formation of single- phased La0.97-xAlO3: xEu3+/ 0.03Tb3+ (x = 0.07), co- doped nanophosphor at 800°C. The synthesized nanophosphors were crystallized in cubic crystal system having Pm3̄m space group with 221 space group number. The morphological studies i.e., field emission scanning electron microscopy (FE- SEM), and transmission electron microscope (TEM) images depicted the agglomerated clusters of distinct spherical shaped particles of La0.97-xAlO3: xEu3+/ 0.03Tb3+ in nano- regime. Energy dispersive X- ray analysis (EDAX) was employed to ascertain the real elemental mapping of the fabricated phosphors. Through diffuse reflectance (DR) spectroscopy measurements, the optical band gap value for La0.92Eu0.05Tb0.03AlO3 nanocrystalline phosphor was determined to be 5.26 eV. The photoluminescent excitation (PLE) and photoluminescent emission (PL) spectra were studied in detail as a function of Eu3+ ion contents and La1-x-0.03AlO3: xEu3+/ 0.03Tb3+ (x = 0.05 mol) co- doped sample exhibits strongest emission and over the 0.05 Eu3+ ions doping concentration, the emission intensity falls as a consequence of the quenching phenomenon. The concentration quenching in directed co- doped nanophosphors was attributed to the dipole - dipole interactions. With the exploitation of photoluminescent data, Commission International de I'Eclairage 1931 (CIE) color coordinates (x, y) of co- doped samples have been calculated from the emission spectra, which revealed the color could be tuned i.e., from orange to red region in La0.97-xAlO3: xEu3+/ 0.03Tb3+ samples with divergences in the Eu3+ and other significant photometric assets viz. correlated color temperature (CCT), color purity (CP) of the synthesized La1-x-yAlO3: xEu3+, yTb3+ co- doped nanocrystalline photoluminescent materials were also determined. The studies outcomes suggested that Eu3+/ Tb3+ co- doped LaAlO3 phosphors have great potential as color- tunable luminescent material in solid- state lighting and display technologies.