In order to enhance micro-computer tomography (micro-CT) imaging of corrosion casts of fine vasculature, metals can be added to the casting resin before perfusion. However, perfused metals lead to vasoconstriction or vessel damage resulting in nonphysiologic vascular casts. A novel method for coating methyl methacrylate vascular casts with osmium tetroxide has been developed in order to increase micro-CT contrast without affecting the vascular structure. This technique was verified using corrosion casts of the lung vasculature of New Zealand white rabbits. Osmium tetroxide coating of methyl methacrylate vascular corrosion casts resulted in an increase in overall sample contrast that translated into an increase in the resolution of the vasculature. This method can therefore lead to increased resolution in the characterization of fine vascular structures.