Shape‐Preserving Chemical Conversion of Architected Nanocomposites

Forging customizable compounds into arbitrary shapes and structures has the potential to revolutionize functional materials, where independent control over shape and composition is essential. Current self‐assembly strategies allow impressive levels of control over either shape or composition, but not both, as self‐assembly inherently entangles shape and composition. Herein, independent control over shape and composition is achieved by chemical conversion reactions on nanocrystals, which are first self‐assembled in nanocomposites with programmable microscopic shapes. The multiscale character of nanocomposites is crucial: nanocrystals (5–50 nm) offer enhanced chemical reactivity, while the composite layout accommodates volume changes of the nanocrystals (≈25%), which together leads to complete chemical conversion with full shape preservation. These reactions are surprisingly materials agnostic, allowing a large diversity of chemical pathways, and development of conversion pathways yielding a wide selection of shape‐controlled transition metal chalcogenides (cadmium, manganese, iron, and nickel oxides and sulfides). Finally, the versatility and application potential of this strategy is demonstrated by assembling: 1) a scalable and highly reactive nickel catalyst for the dry reforming of butane, 2) an agile magnetic‐controlled particle, and 3) an electron‐beam‐controlled reversible microactuator with sub‐micrometer precision. Previously unimaginable customization of shape and composition is now achievable for assembling advanced functional components.