Deduced from thermodynamics and the Thomson Gibbs equation that the surface energy of crystal face is in proportion to the supersaturation of crystal growth units during the crystal growth, we propose that the exposed crystal faces can be simply tuned by controlling the supersaturation, and higher supersaturation will result in the formation of crystallites with higher surface-energy faces. We have successfully applied it for the growth of ionic (NaCl), molecular (TBPe), and metallic (Au, Pd) micro/nanocrystals with high-surface-energy faces. The above proposed strategy can be rationally designed to synthesize micro/nanocrystals with specific crystal faces and functionality toward specific applications.