A comprehensive investigation on the spectroscopic properties and laser performance of Nd3+ doped GdLiF4 (GLF), a new laser crystal, is reported. Our high resolution absorption and emission spectra for GLF are nearly identical to those of Nd:LiYF4 (YLF), a well known laser crystal, strongly suggesting that the two crystals are isostructural. The laser performance of Nd:GLF is very similar to that of Nd:YLF. A maximum laser‐pump‐laser slope efficiency of 68% and 67% was obtained for low (1.0 at. %) and high (4.0 at. %) Nd concentration GLF respectively. Concentration quenching of the fluorescence decay time was observed and appears to be due to the dipole‐dipole interaction between the isolated Nd3+ ions and Nd3+ ion pairs.