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In this work, we demonstrate the systematic and delicate geometry control of Cu2O nanocrystals by taking advantage of the selective surface stabilization effect. A variety of Cu2O architectures, evolved from cubes through truncated cubes, cubooctahedrons, truncated octahedrons and finally to octahedrons, were achieved by simply adjusting the added PVP. Based on the understanding of the intrinsic structural features of the cuprite Cu2O and PVP, we elucidated the underlying shape evolution mechanism. The as-prepared products demonstrated a crystallography-dependent adsorption ability with methyl orange (MeO) as the pollutant. With the advantage of a low cost, high yield and straightforward procedure without pre-formed crystals as sacrificial templates, this method may provide a good starting point for the study of shape construction and morphology-dependent properties of other nanocrystals.