Quasi-crystals, being brittle and porous in bulk form, are usually prepared as coatings, especially using thermal spraying for practical applications. However, due to the strict requirements for the formation of quasi-crystalline phases, powder composition, oxidization, spraying parameter, and heat treatment condition are all involved, which makes the preparation of high purity quasi-crystalline coatings quite difficult. Among the many thermal spraying techniques, high-velocity oxy-fuel spraying (HVOF) should be a good choice for such a purpose as it has a low heat-source temperature and a high particle projection speed, which can effectively avoid the oxidation of quasi-crystalline particles, reduce the ablation of the component metals of quasi-crystalline alloys, and improve the compactness and bonding strength of the coatings. In this article, high purity quasi-crystalline coatings are prepared using HVOF process. Besides the spraying process, heat treatments are specially focused to unveil the effects of different post-annealings on the content of quasi-crystalline phase, microstructure, hardness, and corrosion resistance of the prepared coatings.