The invention provides an Mg-based composite hydrogen storage material containing alkaline earth metals-aluminum hydride and a preparation method thereof, which belongs to the technical field of hydrogen storage material. The chemical general formula of the hydrogen storage material is MgH2+x wt.%(Sr1-yCay)2AlH7+z wt.%TiF3, wherein x is more than or equal to 30 and less than or equal to 50, y is more than or equal to 0 and less than or equal to 0.5, and z is more than or equal to 2 and less than or equal to 10. The hydrogen storage material is gained by mechanically ball milling three materials powder of MgH2, (Sr, Ca)2AlH7 and TiF3, a planetary ball mill is adopted when ball milling, the ball material ratio is 15:1 to 20:1, the rotational speed is 350 to 400rpm, the ball milling time is 10 to 20h, the ball milling protecting atmosphere is argon gas or hydrogen gas, and the atmosphere pressure is 1 to 5atm. The invention has the advantages that: the preparation technique is simple, the provided composite hydrogen storage materials do not need to be activated, and have high hydrogen storage capacity, simultaneously have good low temperature hydrogen absorption dynamic performance and high hydrogen absorption and desorption cycling stability. The invention is applicable to the safe and efficient storage and transportation of the hydrogen, especially the hydrogen fuel cells and other fields.