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To overcome this issue, the electron acceptor molecule 1,2,4,5\u2010tetracyanobenzene (TCNB) was introduced to trigger intermolecular \u03c0\u2013\u03c0 interaction in 2D perovskite along with the electronic doping of 2D\/3D perovskite to improve charge transfer efficiency. By virtue of high electron affinity, TCNB can undergo electron transfer reaction and subsequently establish \u03c0\u2013\u03c0 interaction with 1\u2010naphthalenemethylammonium (NMA) cations, greatly strengthening lattice rigidity and reducing exciton binding energy. Transmission electron microscopy results demonstrate that 2D phases are mainly distributed at grain boundaries, reducing defect density and weakening nonradiative recombination. Meanwhile, the p\u2010type doping of perovskite by TCNB optimizes energy level alignment at perovskite\/hole transport layer interface. Consequently, PCE of champion device is significantly boosted to 24.01\u2009%. The unencapsulated device retains an initial efficiency close to 94\u2009% after exposure to ambient environment for over 1000\u2005h. This work paves a novel path for designing new mixed\u2010dimensional perovskite solar cells with high PCE and superior stability.<\/jats:p>","DOI":"10.1002\/anie.202304256","type":"journal-article","created":{"date-parts":[[2023,4,26]],"date-time":"2023-04-26T11:05:34Z","timestamp":1682507134000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":29,"title":["Electron Acceptor Molecule Doping Induced \u03c0\u2013\u03c0 Interaction to Promote Charge Transport Kinetics for Efficient and Stable 2D\/3D Perovskite Solar Cells"],"prefix":"10.1002","volume":"62","author":[{"given":"Lian","family":"Wang","sequence":"first","affiliation":[{"name":"Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials Ministry of Education School of Materials Science and Engineering Shandong University  250061 Jinan 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