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Vanadium dioxide (VO2) is a much‐discussed material for oxide electronics and neuromorphic computing applications. Here, heteroepitaxy of VO2 is realized on top of oxide nanosheets that cover either the amorphous silicon dioxide surfaces of Si substrates or X‐ray transparent silicon nitride membranes. The out‐of‐plane orientation of the VO2 thin films is controlled at will between (011)M1/(110)R and...