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However, the one\u2010step synthesis of hierarchical asymmetric architectures with precisely controlled morphology and high\u2010curvature interfaces remains challenging. Here, we propose a solvent\u2010driven dissolution\u2010regrowth\u2010migration (SDM) strategy that directs the growth of phenolic resin and regulates the water\u2010oil interface, enabling the one\u2010pot fabrication of asymmetric polymeric and carbon nanoparticles consisting of a mesoporous nanosphere \u201chead\u201d and highly curved lamellar nanosheet \u201ctail\u201d. This SDM process integrates bottom\u2010up self\u2010assembly with top\u2010down selective etching and repolymerization, achieving an \u201cinternal\u2010external synergy\u201d that precisely tailors the surface migration process and asymmetric nanoarchitecture by simply tuning the ethanol content. The asymmetric carbon electrocatalyst, ACN\u2010PdCu, possesses a higher specific surface area, uniformly dispersed PdCu alloy phases, and an elevated Cu\n                    <jats:sup>0<\/jats:sup>\n                    \/Cu\n                    <jats:sup>\u03b4<\/jats:sup>\n                    <jats:sup>+<\/jats:sup>\n                    ratio compared with conventional symmetric nanoparticles. Finite\u2010element simulations and theoretical calculations uncover that this asymmetric architecture enhances local mass diffusion, strengthens substrate adsorption and activation, as well as facilitates charge transfer, thereby improving overall catalytic performance toward the electrocatalytic semihydrogenation of 3\u2010butyne\u20101\u2010ol, achieving &gt;92% conversion and &gt;98% selectivity to 3\u2010butene\u20101\u2010ol, along with excellent cycling stability. The SDM strategy opens a new avenue for designing asymmetric architectures and advanced functional materials with enhanced catalytic activities.\n                  <\/jats:p>","DOI":"10.1002\/adma.72988","type":"journal-article","created":{"date-parts":[[2026,4,8]],"date-time":"2026-04-08T09:26:11Z","timestamp":1775640371000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Solvent\u2010Driven Dissolution\u2010Regrowth\u2010Migration Synthesis of Asymmetric Carbon Nanoparticles for Electrocatalytic Semihydrogenation"],"prefix":"10.1002","volume":"38","author":[{"given":"Lili","family":"Chen","sequence":"first","affiliation":[{"name":"College of Chemistry and Chemical Engineering Inner Mongolia Key Laboratory of Rare Earth Catalysis Institute for Green Chemistry and Environmental Science Inner Mongolia University  Hohhot P. R. 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