The synthesis, physical properties, and molecular structure of (N2C3H)+[Mo2(μ-CH3CO2)[CH3Ga(N2C3H3)O]4]−•2(C4H8O) are reported. Crystals of pyrazolium (μ-acetato)[1,3,5,7-tetramethyl-1,3,5,7-tetrakis(pyrazol-1-yl)cyclotetragalloxanato(4−)]dimolybdate(II)-bis(tetrahydrofuran) are orthorhombic, a = 10.638(2), b = 32.779(4), c = 12.617(1) Å, Z = 4, space group Cmcm. The structure was solved by Patterson and Fourier syntheses and was refined by full-matrix least-squares procedures to R = 0.032 and Rw = 0.041 for 1957 reflections with I ≥ 3σ(I). The structure consists of THF molecules and (N2C3H5)+[Mo2(μ-CH3CO2)[CH3Ga(N2C3H3)O]4]− ion-pair units, the latter displaying exact C2v symmetry. The pyrazolium cation is joined to the complex anion by a pair of strong [Formula: see text] hydrogen bonds [Formula: see text]. The Mo24+ unit is bridged by a single acetato group, the remaining coordination sites being occupied by the hexadentate bridging and chelating [CH3Ga(N2C3H3)O]44− ligand. Bond lengths are: Mo—Mo = 2.127(I), Mo—N = 2.151(3), Mo—O = 2.090(4) and 2.115(4), Ga—O = 1.853(2) and 1.861(2), Ga—N = 1.961(3), and Ga—C = 1.950(6) Å.