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Herein, we report a novel interfacial engineering strategy that employs fullerene C\n                    <jats:sub>60<\/jats:sub>\n                    \u2010mediated\n                    <jats:italic>d\u2010\u03c0<\/jats:italic>\n                    conjugation within a Nb\n                    <jats:sub>2<\/jats:sub>\n                    C\/Nb\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>5<\/jats:sub>\n                    heterostructure (denoted as C\n                    <jats:sub>60<\/jats:sub>\n                    \u2010Nb\n                    <jats:sub>2<\/jats:sub>\n                    C\/Nb\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>5<\/jats:sub>\n                    ) to realize simultaneous electronic reconstruction and structural optimization. The introduced C\n                    <jats:sub>60<\/jats:sub>\n                    forms robust\n                    <jats:italic>d\u2010\u03c0<\/jats:italic>\n                    conjugation with the\n                    <jats:italic>d<\/jats:italic>\n                    \u2010orbitals of Nb, acting as an electron acceptor to drive directional charge transfer across both the C\n                    <jats:sub>60<\/jats:sub>\n                    \/Nb\n                    <jats:sub>2<\/jats:sub>\n                    C and Nb\n                    <jats:sub>2<\/jats:sub>\n                    C\/Nb\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>5<\/jats:sub>\n                    interfaces. Combined theoretical and experimental analyses confirm that orbital engineering between Nb (\n                    <jats:italic>\n                      d\n                      <jats:sub>xy<\/jats:sub>\n                    <\/jats:italic>\n                    \/\n                    <jats:italic>\n                      d\n                      <jats:sub>yz<\/jats:sub>\n                    <\/jats:italic>\n                    ) and C\n                    <jats:sub>60<\/jats:sub>\n                    (\n                    <jats:italic>p<\/jats:italic>\n                    ) facilitates electron backflow, improves intrinsic electronic conductivity, substantially lowers the Li\n                    <jats:sup>+<\/jats:sup>\n                    adsorption barrier, triggers an upward shift of the\n                    <jats:italic>d<\/jats:italic>\n                    \u2010band center, and accelerates electron\u2010transfer kinetics. Consequently, the C\n                    <jats:sub>60<\/jats:sub>\n                    \u2010Nb\n                    <jats:sub>2<\/jats:sub>\n                    C\/Nb\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>5<\/jats:sub>\n                    anode delivers a remarkable reversible capacity of 658.8 mAh g\u2212\n                    <jats:sup>1<\/jats:sup>\n                    at 0.1 A g\u2212\n                    <jats:sup>1<\/jats:sup>\n                    and excellent rate capability. The assembled C\n                    <jats:sub>60<\/jats:sub>\n                    \u2010Nb\n                    <jats:sub>2<\/jats:sub>\n                    C\/Nb\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>5<\/jats:sub>\n                    \/\/activated carbon LIHC achieves a high energy density of 199.5\u00a0Wh kg\u2212\n                    <jats:sup>1<\/jats:sup>\n                    , ranking among the highest values reported for MXene\u2010based LIHCs. This work elucidates a molecular\u2010mediated interfacial electronic engineering mechanism for tailoring charge\u2010storage behavior, providing a rational design strategy for advanced electrochemical energy\u2010storage systems.\n                  <\/jats:p>","DOI":"10.1002\/anie.5198340","type":"journal-article","created":{"date-parts":[[2026,9,23]],"date-time":"2026-09-23T03:46:01Z","timestamp":1790135161000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["C\n                    <sub>60<\/sub>\n                    \u2010Mediated\n                    <i>d\u2010\u03c0<\/i>\n                    Conjugation Induces Electronic Reconstruction to Boost Charge Storage of Nb\n                    <sub>2<\/sub>\n                    C\/Nb\n                    <sub>2<\/sub>\n                    O\n                    <sub>5<\/sub>\n                    Heterostructure Anode"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-6511-2914","authenticated-orcid":false,"given":"Mingming","family":"Gao","sequence":"first","affiliation":[{"name":"State Key Laboratory of New Textile Materials and Advanced Processing School of Materials Science and Engineering Huazhong University of Science and Technology  Wuhan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jundong","family":"Shao","sequence":"additional","affiliation":[{"name":"State Key Laboratory of New Textile Materials and Advanced Processing School of Materials Science and Engineering Huazhong University of Science and Technology  Wuhan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junke","family":"Li","sequence":"additional","affiliation":[{"name":"State Key Laboratory of New Textile Materials and Advanced Processing School of Materials Science and Engineering Huazhong University of Science and Technology  Wuhan 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