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Comprehensive theoretical and experimental studies are performed to discover a new way of synthesis of HfTaC coatings. Here, an evolutionary search for stable crystal structures in the ternary HfTaC system with subsequent selective large‐scale experimental synthesis of coatings using a unique plasma dynamic experimental setup is performed. Optimization of the experimental process allows us to perform selective synthesis of coatings made of hafnium–tantalum carbides with predefined stoichiometry, crystal structure, and properties. Along with more than 70 compounds, the HfTaC system belongs to ternary and quaternary carbides of group IV and V transition metals, and this study opens the door to synthesis of a large number of functional coatings composed of other carbides including high‐entropy carbides.

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