The reduction of energy offsets between donors and acceptors is a direct way to improve the open-circuit voltage (VOC) and overall performance of organic solar cells (OSCs). In this work, two nonfullerene acceptors (NFAs) (BDTBO-4F and BDTBO-4Cl) were synthesized, which were composed of a heptacyclic S,N-heteroacene core and terminal units with halogen atoms, where the latter modulates the energy level of the frontier molecular orbital. Consequently, BDTBO-4Cl exhibited a deeper highest occupied molecular orbital level (EHOMO) and lowest unoccupied molecular orbital level (ELUMO) than BDTBO-4F. Moreover, these two NFAs exhibited high electron mobility and strong absorption at 700-900 nm. The polymer donor PM6 was combined with BDTBO-4F and BDTBO-4Cl, and the resulting OSCs exhibited outstanding power conversion efficiencies of 14.83% for the PM6:BDTBO-4F device and 13.87% for the PM6:BDTBO-4Cl device. More encouragingly, these OSCs exhibited efficient hole transfer from NFAs to PM6, despite small ΔEHOMO(D-A) values (<0.10 eV). These results prove that modulation of EHOMO of acceptors to decrease ΔEHOMO(D-A) is an efficient strategy for high-performance OSCs.