Description:
<jats:title>Abstract</jats:title><jats:p>Significant progress in solar‐cell research is currently made by the development of metal–organic perovskites (MOPs) owing to their superior properties, such as high absorption coefficients and effective transport of photogenerated charges. As for other semiconductors, it is expected that the properties of MOPs may be significantly improved by a defined nanostructure. However, their chemical sensitivity (e.g., towards hydrolysis) prohibits the application of methods already known for the synthesis of other nanomaterials. A new and general method for the synthesis of various (CH<jats:sub>3</jats:sub>NH<jats:sub>3</jats:sub>)PbI<jats:sub>3</jats:sub> nanostructures from a novel single‐source precursor is presented. Nanoporous MOP single crystals are obtained by a crystal‐to‐crystal transformation that is accompanied by spinodal demixing of the triethylene glycol containing precursor structure. Selective binding of a capping agent can be used to tune the particle shape of the MOP nanocrystals.</jats:p>