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Unfortunately, their practical performance is often compromised by hydration\u2010induced membrane swelling, giving rise to non\u2010selective water channels that facilitate catholyte\u2010anolyte crossover. Herein, we show that geometric topology is a previously overlooked but decisive parameter governing membrane microstructure, hydration behavior, and ion selectivity. Using a coarse\u2010grained molecular dynamics framework, we reveal a geometry\u2010driven phase\u2010separation mechanism under membrane hydration. Isotropic 0D geometric motifs remain uniformly dispersed and promote the formation of highly interconnected yet spatially confined hydration networks, whereas anisotropic one\u2010 and 2D geometric motifs exhibit a strong propensity to bundle and aggregate, inducing phase separation and interfacial voids that promote non\u2010selective transport. Guided by this principle, a membrane incorporating 0D geometric motifs simultaneously achieves high cationic conductivity and strong polysulfide rejection, enabling stable operation of a polysulfide\u2010based aqueous redox flow battery for over 700 h with Coulombic efficiencies exceeding \u223c99.5% and peak power densities of \u223c138\u00a0mW cm\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>2<\/jats:sup>\n                    , dramatically outperforming conventional commercial membranes and demonstrating the effectiveness of the geometry\u2010guided membrane design principle in advancing future membrane engineering.\n                  <\/jats:p>","DOI":"10.1002\/adma.73904","type":"journal-article","created":{"date-parts":[[2026,7,4]],"date-time":"2026-07-04T15:39:41Z","timestamp":1783179581000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Geometric\u2010Topology\u2010Driven 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