Single-phased cool white light emissive Gd3-xAl5O12:xDy3+ (x = 0.01–0.07) nanophosphors have been prepared via gel-combustion method. Diffraction data and Rietveld results have affirmed the development of a single cubic phase of all the prepared samples with space group Ia-3d (230). Furthermore, the crystallite size was calculated through Debye-Scherrer's formula and the Williamson-Hall method. In the EDX spectrum, the nonappearance of peaks analogous to the foreign elements affirms the pure synthesis of the considered phosphors. TEM observation reveals agglomerated porous crystalline material with non-uniform shapes and varying particle size in 20–80 nm range. Fourier Transform Infrared (FTIR) spectroscopy has been applied for the examination of chemical bonding with other vibrational characteristics. The luminescence study confirms the intense blue and yellow emission of synthesized phosphors at 482 nm and 576 nm respectively owing to 4F9/2→6HJ (J = 15/2, 13/2) transitions. Moreover, the detailed evaluation of the concentration quenching process established that dipole-quadruple interaction is answerable for the decrease in luminescence intensity after optimum dopant ion concentration. The chromatic analyses recommend that emission from the optimized nanophosphors lies in the region of cool white light. The outcomes of the present investigation propose that Gd3Al5O12:Dy3+ phosphors might be a potential candidate for white-LEDs applications.