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Auxetic-like strain states were generated in self-assembled nanocomposite thin films of (Ba 0.6 Sr 0.4 TiO 3) 1− x−(Sm 2 O 3) x (BSTO− SmO). A switch from auxetic-like to elastic-like strain behavior was observed for x> 0.50, when the SmO switched from being nanopillars in the BSTO matrix to being the matrix with BSTO nanopillars embedded in it. A simple model was adopted to explain how in-plane strain varies with x. At high x (0.75), strongly enhanced ferroelectric properties were obtained compared to pure BSTO films. The nanocomposite method represents a powerful new way to tune the properties of a wide range of strongly correlated metal oxides whose properties are very sensitive to strain.