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Herein, we report two novel solid additives of BQ and BBQ, which feature a D\u2010A\u2010D type 2,5\u2010di(thiophen\u20102\u2010yl)pyrazine conjugated skeleton, to regulate the D18 donor layer in D18\/L8\u2010BO devices. The BQ molecule contains carbamate side chains that form robust intramolecular hydrogen bonds with the pyrazine core, locking the backbone into a planar and pseudo\u2010pentacyclic structure. This structural feature enhances the crystallinity and face\u2010on orientation of D18 film, fostering an optimized fibrillar network. This network acts as an ideal scaffold for subsequent deposition of L8\u2010BO, thus resulting in a pseudo\u2010bulk heterojunction with expanded interfacial area for exciton dissociation and continuous channels for charge transport. Consequently, the BQ\u2010processed LbL\u2010OSCs achieve an impressive efficiency of 20.29%. In contrast, the brominated analogue BBQ exhibited relatively excessive phase separation, which disrupted the active layer homogeneity and hindered optimal molecular packing. This work highlights the efficacy of hydrogen\u2010bond\u2010mediated solid additives in fine\u2010tuning the morphology of the donor layer for high\u2010performance LbL\u2010OSCs.<\/jats:p>","DOI":"10.1002\/smll.73977","type":"journal-article","created":{"date-parts":[[2026,5,26]],"date-time":"2026-05-26T10:07:39Z","timestamp":1779790059000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Hydrogen\u2010Bond\u2010Mediated Solid Additives Enabling Enhanced Bi\u2010Continuous Interpenetrating Network for 20.29% Efficiency Layer\u2010by\u2010Layer Organic Solar Cells"],"prefix":"10.1002","volume":"22","author":[{"given":"Zhentao","family":"Hu","sequence":"first","affiliation":[{"name":"School of Chemical Engineering and State Key Laboratory of Advanced Polymer Materials Sichuan University  Chengdu P. R. 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