Two cobalt compounds, Cp*Co(CO)I2 (1) and CpCo(CO)I2 (2) (Cp* = η(5)-C5Me5, Cp = η(5)-C5H5), catalyze the dehydrogenation of ammonia borane under either anaerobic or aerobic conditions and are also effective hydrogenation catalysts for alkenes and alkynes using ammonia borane as a hydrogen source, also in the presence of air.