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By employing the asymmetric end‐group engineering, an asymmetric nonfused‐ring electron acceptor (NFREA) was designed and synthesized. Compared with the symmetric analogs (NoCA‐17 and NoCA‐18), NoCA‐19 possesses broader light absorption range, more coplanar π‐conjugated backbone, and appropriate crystallinity according to the experimental and theoretical results. The organic solar cells based on J52:NoCA‐19...