A quadruply bonded dimolybdenum complex with trans-crotonate ligands, Mo2(O2CC3H5)4, was synthesized and characterized by UV–VIS, IR, and NMR spectra. The crystal structure was determined by an X-ray single crystal diffraction analysis. The title complex (C16H20O8Mo2, M w = 532.2) crystallized in the triclinic space group P-1 with the following crystallographic parameters: a = 10.236(2) Å, b = 10.393(2) Å, c = 10.524(2) Å, α = 89.59(1)°, β = 73.34(1)°, γ = 70.78(2)°, V = 1008.1(3) Å3, Z = 2, D c = 1.753 Mg m−3, μ(Mo Kα = 0.71073 Å, F(000) = 528, and final R 1 = 0.041, wR 2 = 0.114 for observed reflections 2889 (I > 2σ(I)). The Mo2 4+ unit was surrounded by four trans-crotonate ligands resulting in a paddle wheel structure with one disordered trans-crotonate ligand. Molecules are bonded together by means of interactions consisting of the donation of lone pairs of electron on carboxylate O atoms on one molecule to the Mo atom on an adjacent complex. A new pattern of intermolecular bonding is observed.