Single crystals of molybdenum-oxy-di-tetrahydrouran-trichloride were obtained by the reaction of Mo2Cl10, tetrahydrofuran, sulfur, and P4S3 in carbon disulfide after layering the solution with n-hexane. Single crystal structure determination at T = 123 K reveals that MoOCl3(THF)(2) crystalizes in the orthorhombic space group P2(1)2(1)2(1) with the lattice constants a = 7.8620(9) angstrom, b = 12.302(1) angstrom, c = 14.043(2) angstrom, V = 1304.10(3) angstrom(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.