The effect of co-doping Y3+ and the doping concentration of Nd3+ on the spectroscopic properties and laser performance of Nd:CaF2 crystals are investigated systematically. For a 0.5% Nd:CaF2 crystal, the emission lifetime at 1.06 μm increases from 18 to 361 μs by co-doping 10 at.% Y3+, while the emission cross section increases to 4.27×10 20 cm2 at 1054 nm. With a 10 at.% doping concentration of Y3+, Nd,Y:CaF2 crystals concentrate emission bands that peak at 1054 nm with shoulders at 1063 nm, and FWHM at about 30 nm. A diode-pumped, highly efficient laser operation is obtained with 0.5% Nd, 10% Y:CaF2 and 0.6% Nd, 10% Y:CaF2 crystals, with slope efficiencies over 30% and 27%, respectively, and a maximum output power up to 901 mW.