Electron paramagnetic resonance spectra of homoleptic and mixed-ligand molybdenum tris(dithiolene) complex anions [Mo(tfd)(m)(bdt)(n)](-)(n + m = 3; bdt = S2C6H4; tfd = S2C2(CF3)(2)) reveal that the spin density has mixed metal ligand character with more ligand-based spin for [Mo(tfd)3](-) and a higher degree of metal-based spin for [Mo(bdt)(3)](-): the magnitude of the isotropic Mo-95,Mo-97 hyperfine interaction increases continuously, by a factor of 2.5, on going from the former to the latter. The mixed complexes fall in between, and the metal character of the spin increases with the bdt content. The experiments were corroborated by density functional theory computations, which reproduce this steady increase in metal-based character.