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Regulating the intermolecular interaction to disperse the aggregation and further improve the molecular packing order of SMAs would be an effective strategy to solve this problem. Here, we designed and synthesized two SMAs L8\u2010PhF and L8\u2010PhMe by introducing different substituents (fluorine for L8\u2010PhF and methyl for L8\u2010PhMe) on the phenyl end group of the inner side chains of L8\u2010Ph, and investigated the effect of the substituents on the intermolecular interaction of SMAs,\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>loss<\/jats:sub>\n                    and performance of OSCs processed with non\u2010halogenated solvents. Through single crystal analysis and theoretical calculations, it is found that compared with L8\u2010PhF, which possesses strong and abundant intermolecular interactions but downgraded molecular packing order, L8\u2010PhMe with the methyl substituent possesses more effective non\u2010covalent interactions, which improves the tightness and order of molecular packing. When blending the SMAs with polymer donor PM6, the differences in intermolecular interactions of the SMAs influenced the film formation process and phase separation of the blend films. The L8\u2010PhMe based blend film exhibits shorten film formation and more homogeneous phase separation than those of the L8\u2010PhF and L8\u2010Ph based ones. Especially, the OSCs based on L8\u2010PhMe show reduced non\u2010radiative energy loss and enhanced\n                    <jats:italic>V<\/jats:italic>\n                    <jats:sub>oc<\/jats:sub>\n                    than the devices based on the other two SMAs. Consequently, the L8\u2010PhMe based device processed with\n                    <jats:italic>o<\/jats:italic>\n                    \u2010xylene (\n                    <jats:italic>o<\/jats:italic>\n                    \u2010XY) and using 2PACz as the hole transport layer (HTL) shows an outstanding PCE of 19.27\u2009%. This study highlights that the\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>loss<\/jats:sub>\n                    of OSCs processed with non\u2010halogenated solvents could be decreased through regulating the intermolecular interactions of SMAs by inner side chain modification, and also emphasize the importance of effectivity rather than intensity of non\u2010covalent interactions introduced in SMAs on the molecular packing, morphology and PCE of OSCs.\n                  <\/jats:p>","DOI":"10.1002\/anie.202416016","type":"journal-article","created":{"date-parts":[[2024,9,25]],"date-time":"2024-09-25T09:48:53Z","timestamp":1727257733000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":43,"title":["Inner Side Chain Modification of Small Molecule Acceptors Enables Lower Energy Loss and High Efficiency of Organic Solar Cells Processed with Non\u2010halogenated 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