During the deposition of Cr3C2-NiCr coatings, compositional degradation occurs, primarily through the dissolution of the carbide phase into the matrix. Exposure at an elevated temperature leads to transformations in the compositional distribution and microstructure. While these have been investigated in short-term trials, no systematic investigations of the long-term microstructural development have been presented for high-velocity sprayed coatings. In this work, high-velocity air fuel (HVAF) and high-velocity oxygen fuel (HVOF) coatings were treated at 900 °C for up to 60 days. Rapid refinement of the supersaturated matrix phase occurred, with the degree of matrix phase alloying continuing to decrease over the following 20 to 40 days. Carbide nucleation in the HVAF coatings occurred preferentially on the retained carbide grains, while that in the HVOF coatings developed in the regions of greatest carbide dissolution. This difference resulted in a variation in carbide morphologies. Preferential horizontal growth was evident in both coatings over the first 20 to 30 days of exposure, beyond which spheroidization of the microstructure occurred. After 30 days, the carbide morphology of both coatings was comparable, tending toward an expansive structure of coalesced carbide grains. The development of the carbide phase played a significant role in the microhardness variation of these coatings with time.