We demonstrate a novel synthetic scheme that can be used to differentially guide the shape of PbS semiconductor nanocrystals. Our study first demonstrates the discovery of single-crystalline star-shaped nanocrystals as novel transient species. We then carefully probe their shape evolution toward other novel nanostructures (e.g., tadpole-, L-, T-, cross-shapes, highly faceted star shapes, truncated octahedrons and cubes, etc.) and systematically elucidate the key parameters that control these final structures. In principle, through programming these growth parameters, the desired architecture of building blocks of other kinds of nano materials can be constructed.

The systematic shape control of colloidal nanocrystals including one‐dimensional (1D) nanorods remains a key issue in the “bottom–up” approach of nanoscience. Here, we examine the anisotropic structural evolution of various semiconductor nanocrystals and systematically elucidate the key growth parameters for their shape control. The crystalline phase of nucleating seeds and kinetic growth regimes controlled by changing growth parameters are crucial for the determination of the 1D nanocrystal geometry.

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