Cr-Ga-N thin films were prepared on (100)-oriented MgO single-crystal substrates by pulsed laser deposition at various substrate temperatures. An ablation plasma, generated by irradiating a Cr-10 at. % Ga alloy target with a Nd:YAG laser, was applied to the substrates to deposit the Cr-Ga-N thin films. Rutherford backscattering spectroscopy revealed that the ratio of the amount of Ga to the amount of Cr plus Ga (hereafter Cr+Ga) in all Cr-Ga-N thin films was approximately 10 at. %. X-ray diffraction and microstructural observation indicated that Cr-Ga-N thin films deposited at substrate temperatures (T sub ) above 773 K contained two crystal phases: B1 (NaCl type)-CrN and B4 (würtzite type)-GaN. By contrast, Cr-Ga-N thin films deposited at a T sub of 673 K grew epitaxially and were composed of a single B1-(Cr,Ga)N phase, synthesized by substituting some of the Cr atoms in B1-CrN with Ga atoms. The epitaxial B1-(Cr,Ga)N thin films showed a higher hardness than epitaxial CrN films.