We report a new pulsed chemical vapor deposition (PCVD) process to deposit nickel (Ni) and nickel carbide (Ni3C
) thin films, using bis(1,4-di-tert-butyl-1,3-diazabutadienyl)nickel(II) precursor and either H2 gas or H2 plasma as the coreactant, at a temperature from 140 to 250 °C. All the PCVD films are fairly pure with low levels of N and O impurities. The films deposited with H2 gas at ≤200 °C are faced centered cubic-phase Ni metal films with low C content; but at ≥220 °C, another phase of rhombohedral Ni3C is formed and the C content increases. However, when H2 plasma is used, the films are always in rhombohedral Ni3C phase for the entire temperature range.