We report the first tris(alkoxide)V(III) complex to bind dinitrogen. Removal of THF from V(OR)(3)THF furnishes the highly reactive V(OR)(3) fragment, which binds dinitrogen to form [V(OR)(3)](2)(μ-N(2)) in the solid state. Dinitrogen is readily released upon dissolution of the complex. Structural and DFT studies are consistent with significant activation of N(2) when bound by the vanadium tris(alkoxide) platform.