The invention provides tunable laser crystal chrome-doped sodium magnesium molybdate and a preparation method thereof. A molten salt top seed crystal method is adopted, 55-80at.% of Na2Mo2O7 is used as a melting assistant, and the growth parameters are as follows: the cooling velocity is 0.5-3 DEG C/day, the growth temperature is 800-880 DEG C, the rotation speed is 5-30rpm/minute, and a Cr<3+>:Na2Mg5(MoO4)6 crystal which is relatively good in quality and relatively large in size is grown, wherein the doping concentration of Cr<3+> is 0.2-5at.%. The crystal belongs to a triclinic system, and has a P-1 space group structure as shown in the specification. The crystal has the characteristics that the mechanical property is moderate, the tunable laser wave band is wide, the emission cross section is large, and the like, and is a relatively good tunable laser crystal material.