A three-dimensional coordination polymer, {(Mo 2 O 6 )(4,4'-bpy)} n (1) (4,4'-bpy = 4,4'-bipyridine), was synthesized under solvothermal conditions and characterized by single crystal X-ray diffraction analysis, powder X-ray diffraction (XRD), Fourier transformation infrared (FT-IR) spectroscopy and thermogravimetric analysis (TGA). The coordination polymer was also prepared in nanoscale via an ultrasound-assisted top-down process. The nanosized coordination polymer was characterized by means of scanning electron microscopy (SEM), XRD and FT-IR spectroscopy. The prepared oxomolybdate-based coordination polymer, in bulk and nanoscale, was applied as heterogeneous catalyst for the epoxidation of some olefins using tert-butyl hydroperoxide (TBHP) as oxidant. The 3-D coordination polymer, particularly in nanoscale, demonstrated good activity and stability in the epoxidation reaction and could be easily recovered and reused in the reaction.