The studies of the growth mechanism of aluminide coatings by chemical vapor deposition (CVD) is an important prerequisite for optimizing the thermal protection properties of aluminide coatings and improving the CVD process parameters; however, the current research on the growth mechanism of CVD aluminide coatings on nickel-based alloys is relatively limited, and there is a lack of systematic studies in this area. In this work, aluminide coatings were prepared on the surface of nickel-based superalloys by the CVD method, and elemental diffusion and microstructure effects between coating and substrate at different deposition temperatures and times, as well as the growth kinetics and formation mechanism of CVD aluminide coatings were investigated. The results showed that the coating prepared on the surface of K444 nickel-based high-temperature alloy by CVD was an externally diffused aluminide coating with a bilayer structure: the outer layer of the coating was the β-NiAl phase. The interdiffusion layer was mainly composed of nickel-aluminum compounds, carbides, and topologically close-packed phase. The growth of the CVD aluminide coating was mainly controlled by the grain boundary diffusion mechanism.