Nanocrystalline phosphors NaGd1- x Nd x F4 ( x = 0-1) were synthesized by hydrothermal synthesis for the first time. All the synthesized compounds have hexagonal β-NaYF4 crystalline phase. Neodymium(III) ions isomorphically replace gadolinium ions. NaGd0.96Nd0.04F4 compound has the largest photoemission intensity in NIR range upon 808 nm excitation; further doping with Nd3+ results in concentration quenching.