The effect of doping concentration of Nd3+ and co-doping Y3+ on the spectroscopic properties are investigated systematically. Due to the particular clustering effect, the quench effect was demonstrated in lightly doped NdxGd0.03Sr0.97-xF2.03+x (x=0.0005,0.0015,0.0065,0.01) crystals. For a 3% Gd:SrF2 crystal, the fluorescence lifetime at 1054 nm decrease from 380.9 to 159.8 μs by doping Nd3+ from 0.15 at.% to 1 %at.%, while the emission cross section decreases to 4.12 × 10−20cm2 at 1054 nm. However, the absorb cross section were increased when the concentration of Nd3+ increase from 0.5 % to 0.65 %. Thus, there is an optimum doping concentration of Nd3+. According to the research, the optimum doping concentration of Nd3+ is 0.15 % in 3% Gd:SrF2 crystals.