Objective To prepare the MoSi2 coating on the surface of Nb-Ti-Si alloy. Methods The coating was prepared through glow plasma deposition of Mo and pack siliconization. The effects of temperature on the microstructure, thickness and element distribution of the deposited Mo layer were analyzed, and the coating structure of the Mo layer after siliconization was investigated. Results Elements inter-diffusion between the glow plasma deposited Mo layer and the substrate was significant at 1100 ℃; after siliconization, dense MoSi2 coating was formed on the substrate. The MoSi2 coating had a multi-layer structure. From the surface to the substrate, the MoSi2 coating was consisted of the MoSi2 layer, the NbSi2 layer and the Nb5Si3 layer; a (Mo,Nb)Si2 inter-diffusion zone was formed between the MoSi2 layer and the NbSi2 layer. Conclusion The MoSi2 coating could be prepared on the surface of the Nb-Ti-Si alloy through glow plasma deposition of Mo/ pack siliconization. The coating had metallurgical bonding with the substrate.