Engineering of Asymmetric Hollow Carbon Nanoparticles with Tunable Architecture via Flowable Colloidal Polymer‐Emulsion Assembly Strategy

Abstract Asymmetric hollow carbon (AHC) nanoparticles, celebrated for their distinctive external morphology, intricate internal topology, and exceptional carbon performance, are capturing significant attention. Nevertheless, exploring a universal emulsion assembling system to endow them with customizable architectures remains a formidable yet pending challenge. Interestingly, inspired by “plasticization”, a flowable colloidal polymer‐emulsion assembly strategy is first reported. It makes a striking debut of “dynamically growing‐like” AHC architectures, encompassing double‐headed mushroom, pleurotus eryngii, oyster mushroom, mushroom envelope, mushroom cap, and truffle‐shaped. This breakthrough creates an unprecedented “complete coverage” emulsion assembly mode, which surpasses the constraints of conventional “incomplete coverage” mode and infuses fresh vitality into the thriving nanoparticle‐library. More excitingly, it just is a brand‐new mechanism – the synergistic effect of plasticizing and swelling that flexibly manipulates the assembly between size‐variable emulsion droplet templates and flowable colloidal polymer, thereby successfully propelling the reversible architectural evolution. Remarkably, by skillfully integrating double‐headed mushroom‐shaped AHC nanoparticles with PEG and polyurethane sponge to engineer a composite adsorbent with reliable thermophysical property, it can offer a promising avenue for environmental governance. Generally, these cutting‐edge findings not only enrich the theory of emulsion assembly but also spark fresh inspiration for a vast spectrum of potential applications.