The generations of high energy 2nd- and 3rd-order stimulated Raman scattering lasers based on the α-BaTeMo 2 O 9 crystal were demonstrated for the first time. The Raman gain coefficient has been compared with that of the YVO 4 crystal. A maximum total Stokes radiation energy of 27.3mJ was obtained, containing 20.1mJ 2nd-order Stokes energy at 1318nm, together with 7.2mJ 3rd-order Stokes energy at 1497nm, giving an overall conversion efficiency of 35.9% and a slope efficiency of 54.5%. With an optical coating design, a total 3rd- and 4th-order Stokes energy of 16.5mJ was generated. The maximum energy for 4th-order Stokes radiation at 1731nm was 2mJ. The pulse durations for the 2nd-, 3rd-, and 4th-order Stokes shift were 10ns, 8.6ns, and 5.2ns, respectively. Our experimental results show that the α-BTM crystal is a promising Raman crystal for the generations of eye-safe radiations.