In conclusion, we have synthesized ZnGa2O4:Cr3+ powder via a solid-state reaction and subsequently deposited it as a thin film on quartz substrates using a pulsed laser deposition technique under two different deposition conditions. The XRD results show that the sample deposited at an oxygen pressure of 1 Pa (the 1-Pa film sample) is of higher purity and better crystallization than that deposited at an oxygen pressure of 0 Pa (the 0-Pa film sample). The SEM results confirm that ZnGa2O4:Cr3+ films manifest preferred orientation.