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Here, we construct a Cu7S4\/CuCo2S4 heterostructure in a single hydrothermal process, in which the two phases sharing a common Cu\u2013S sublattice form a coherent interface within individual particles. By fixing the phase ratio independently through Rietveld refinement and benchmarking against both phase-pure constituents under identical conditions, we show that the composite exceeds the composition-weighted rule-of-mixtures prediction by a factor of 3.4 at 0.3 A g\u20131. Because the constituents exhibit closely comparable charge\u2013discharge profiles, the redox chemistry itself is unchanged, and this strongly super-additive response can primarily originate from the interface rather than from composition. Elemental mapping and surface-sensitive XPS, together with the coexistence of Li2S and MgS in in situ XRD, further reveal that storage is spatially partitioned: Li+ converts the particle interior while Mg2+ reacts predominantly in the near-surface region, so that the two carriers occupy complementary regions of the same particle. Comparing APC-LiCl with APC-LiTFSI at matched salt concentration, and identical in every other respect, localizes the electrolyte effect to the electrode interface, where the chloride-containing system suppresses the progressive Mg-surface passivation that drives continuous overpotential growth in the TFSI\u2013 system. The resulting cell delivers 400 mAh g\u20131 at 0.3 A g\u20131 and retains 152.56 mAh g\u20131 after 330 cycles at 1.0 A g\u20131 at \u223c100% Coulombic efficiency. DFT calculations indicate increased states near the Fermi level and a localized interfacial electrostatic gradient consistent with the measured kinetics.<\/jats:p>","DOI":"10.1021\/acsami.6c16394","type":"journal-article","created":{"date-parts":[[2026,10,7]],"date-time":"2026-10-07T19:02:09Z","timestamp":1791399729000},"page":"56223-56235","source":"Crossref","is-referenced-by-count":0,"title":["Quantifying the Heterointerface Contribution in a Cu7S4\/CuCo2S4 Cathode with LiCl-All-Phenyl Complex Electrolyte for High-Performance Magnesium\/Lithium Hybrid-Ion Batteries"],"prefix":"10.1021","volume":"18","author":[{"given":"Xuehui","family":"Wang","sequence":"first","affiliation":[{"name":"Anhui Normal University , , , ,","place":["Wuhu, Anhui, P.R. 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