Single crystals of molybdenum-oxy-di-tetrahydrofuran-trichloride were obtained by the reaction of Mo 2 Cl 10 , tetrahydrofuran, sulfur, and P 4 S 3 in carbon disulfide after layering the solution with n-hexane. Single crystal structure determination at T = 123 K reveals that MoOCl 3 (THF) 2 crystalizes in the orthorhombic space group P2 1 2 1 2 1 with the lattice constants a = 7.8620(9) Å , b = 12.302(1) Å , c = 14.043(2) Å , V = 1304.10(3) Å 3 , and Z = 4. EPR experiments on the solid compound showed a g value of 1.94 at 347.46 mT, which accords to a Mo(V) species. The electronic structure of the title compound was investigated with DFT methods.