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KNbO3in the form of films is a highly acclaimed material due to its potential application in surface acoustic wave (SAW), and nonlinear optic devices. Single‐source powder flash evaporation MOCVD of epitaxial KNbO3films was accomplished, for the first time, with potassium tert‐butoxide and niobium heteroligand complex, Nb(OiPr)4(thd) used as volatile metal–organic precursors. The microstructure of the films was found to be dependent on the substrate used (MgO or SrTiO3) and deposition temperature. A new approach to reach cation stoichiometry of deposited films deficient in potassium, consisting of a post‐deposition annealing with a KNbO3/K3NbO4powder mixture, was proposed. The device quality of the films was verified by high second harmonic generation (SHG) output. The effect of the oxygen non‐stoichiometry of films on the phase transition temperature was proven.