VO 2 is a smart transition-metal oxide, which exhibits a tetragonal-to-monoclinic phase transition at ∼ 68°C. We report a case where both tetragonal and monoclinic phases exist in relaxed and strained domains, respectively, above the transition temperature. The epitaxial nucleation of these relaxed domains of VO 2 over the strained one occurs when the critical thickness criterion is met through the emergence of interfacial dislocations under domain-matching epitaxy paradigm. Below this critical thickness, the film isostructurally (across the transition temperature range) adopts a strained-monoclinic phase. Above the critical thickness, domains are structurally free to transform from tetragonal to monoclinic. IMPACT STATEMENT We studied formation and atomic-scale characterization of a novel heterostructure of relaxed (tetragonal/monoclinic) and unrelaxed (monoclinic) VO 2 phases. The monoclinic-to-tetragonal structural transition occurs at the critical thickness of ∼ 15 nm.