NiCr-Mo composite coating was prepared by plasma spraying of shell-core-structured NiCr-Mo powders. The morphologies of the NiCr-Mo powders and microstructure of the corresponding NiCr-Mo coating were characterized by SEM. Furthermore, the erosion behavior of the NiCr-Mo coating at impact angles of both 30° and 90° was investigated, and was further compared with that of the Ni20Cr coating and the In-738 alloy bulk. Results showed that fully-dense and homogenous NiCr-Mo coating with excellent interface bonding and no pure Mo inclusions was obtained. Furthermore, the erosion test results showed that the erosion rate of the optimized NiCr-Mo coating is lower than that of NiCr coating at both impact angles. Moreover, the NiCr-Mo coating presented excellent erosion resistance which was comparable as that of In-738 alloy bulk, attributing to the fully-dense microstructure and metallurgical interface bonding within coating.