The invention discloses a high magnetostrictive Fe-based metal glass magnetic material and a preparation method thereof. The chemical formula of the high magnetostrictive Fe-based metal glass alloy is Fe100-x-y-zMozByTbx, wherein, x, y and z are respectively the atomic percents of Tb, B and Mo, 100-x-y-z is the atomic percent of Fe, x is more than 0 and less than or equal to 10, y is more than or equal to 20 and less than or equal to 25, z is more than 0 and less than or equal to 10. The preparation method of the alloy is as follows: the industrial pure metals Fe, Mo, Tb and FeB alloy are proportioned according to the alloy formula and melted repeatedly by induction-arc under the protection of argon to make master alloy, then the high magnetostrictive Fe-based metal glass magnetic material is obtained through casting by using the copper mold spray-casting method. The magnetostrictive coefficient of the magnetic material is 420 ppm to 985 ppm, and the magnetic material has simple components, high thermal stability, and good mechanical properties and amorphous forming ability. The high magnetostrictive Fe-based metal glass magnetic material can be widely applied to the fields of sonar transducer, sensor, ultrasonic technology, communication technology, and the like.