This invention provides a self-activation laser crystal of tungstic acid neodymium lithium and its method for preparation and usage, which relates to artificial crystals and their growing field. The molecular formula of the crystal is LiNd(WO4)2, belonging to tetragonal system, with space group of I4(1) / a(C4h6) and crystal parameter of a=b=5.2525 ,c=11.3397 ,V=314.43 3,Dc=6.843g / cm3. Using molten salt growth method, taking Li2W2O7 for fluxing agent, in the range of 950-814 degrees, with detemperature rate of 0.5-1 degrees per day, the crystal growing. Crystal grows with lifting and pulling method, which growing temperature of about 1080 degrees, lifting rate of 0.5-0.6 millimeter per hour and crystal rotary rate of 15-30 revolutions per minuten. The crystal used as working-laser material can produce laser output of 1069nm wavelength, and it can be used in laser of spectroscopy, biochemistry, medical treatment and military affairs fields.