Through photoluminescence (PL) investigations, this work shows that the hydrothermal technique of nanomaterial synthesis can successfully produce GdPO4:Nd3+/Ho3+ nanophosphors that display luminescence properties. Down-conversion peaks that produce green and red light arise at certain wavelengths (465, 550, and 674 nm) in response to stimulation at 300 nm. The analysis indicates the P-O CT band of Ho3+ ions and non-radiative resonance energy transfer, which boosts Ho3+ ion emission. GdPO4:Nd3+/Ho3+, an up-conversion (UC) nanophosphor, exhibits efficient luminescence output, with Ho3+ ions being attributed to distinct peaks in the up-conversion emission spectra (465 nm, 550 nm, and 674 nm). Nd3+ ions under strong 808 nm laser irradiation promote these peaks. The study produces well-crystalline nanoparticles with diameters ranging from a few nanometers to tens of nanometers by using the hydrothermal synthesis approach. Under PLE tests, the nanophosphors show an impressive quantum yield, suggesting a wide range of possible uses in the field of nanophosphor materials.