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Nonfullerene acceptors (NFAs) have contributed significantly to the progress of organic solar cells (OSCs). However, most NFAs feature a large fused-ring backbone, which usually requires a tedious multiple-step synthesis, and are not applicable to commercial applications. An alternative strategy is to develop nonfused NFAs, which possess synthetic simplicity and facile tunability in optoelectronic properties and solid-state microstructures. In this work, we report two nonfused NFAs, BTCIC and BTCIC-4Cl, based on an A–D–A′–D–A architecture, which possess the same electron-deficient benzothiadiazole central core but different electron-withdrawing terminal groups. The optical properties, energy levels, and molecular crystallinities were finely tuned by changing the terminal groups. Moreover, a decent power conversion efficiency of 9.3 and 10.5% has been achieved by BTCIC and BTCIC-4Cl, respectively, by …