The new nonlinear optical (NLO) crystal BaGa4S7 for the mid-infrared (IR) has been grown by a Bridgman-Stockbarger technique. Polycrystalline materials with stoichiometric composition were synthesized from BaS, Ga, and S as the initial materials by solid-state reactions. The ultraviolet (UV) and IR transmittance of the crystal was determined with polished crystal pieces. The UV and IR optical absorption edges were found to be at 350 nm and 13.7 μm, respectively. From optical measurements of second harmonic generation on powders, the NLO coefficient d33 was determined to be 12.6 pm/V. The laser damage threshold of a single crystal reached about 1.2 J/cm2 at 1.064 μm. The Vickers-hardness value of the crystal is 327.5 HV5, which is equivalent to Mohs’ hardness of about 5.