The deposition of Co thin films by organometallic chemical vapor deposition is reported. Co is of interest in very large scale integration technology as a catalyst for electroless plating of other metals and as a precursor to formation of CoSi2. High purity, conformal films of Co are deposited by pyrolysis of Co2(CO)8at 200 °C in vacuum. These films exhibit electrical resistivities of 5–10 μΩ cm and excellent adhesion to Si and SiO2. CoSi2is formed by heating the samples at 700 °C. The CoSi2films resulting from reaction of the Co films with the Si substrate contain larger grains than the starting film and exhibit electrical resistivities of ∼13–37 μΩ cm. Selective formation of CoSi2on patterned test wafers shows similar attributes.