| Summary: | Abstract Engineered nanoparticles have emerged as new types of materials for a wide range of applications from therapeutics to energy. Still, fabricating nanomaterials presenting complex inner morphologies and shapes in a simple manner remains a great challenge. Herein, we report the template‐free one‐pot continuous gradient nanoprecipitation of different types of non‐compatible polymers to spontaneously form nanostructured particles. The continuous addition of antisolvent induces precipitation and (re)organization of polymer chains at the forming particle interface, ultimately and naturally developing complex inner morphologies and shapes while particle grows. This low‐energy‐cost bottom‐up assembly approach applies to various functional polymers, possibly embedded with metal nanoparticles, for continuous growth into well‐organized nanoparticles. UV crosslinking of the particles and core removal allows both confirming the building process and leading to hollow or multivoid nanomaterials.
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