A new structurally defined precursor compound for the low‐temperature metalorganic chemical vapor deposition (MOCVD) of CoAs thin films is reported. The easily accessible 1,3‐bis(tert‐butyl)‐2‐[tetracarbonyl‐cobalt(‐l)]‐1,3,2‐diazarsolidine was decomposed by hot‐wall low pressure CVD. Thin films of cobalt arsenide with retention of the stoichiometry of the precursor (Co:As=1/1) were formed at temperatures as low as 210 °C. Electron micrographs show uniform films, energy dispersive x‐ray spectroscopy, and Auger electron spectroscopy confirm their bulk composition, and powder diffraction patterns and conductivity measurements prove their crystallinity and electrical properties. ©1995 American Institute of Physics.