To maximize the short-circuit current density (J(SC)) and the open circuit voltage (V-OC) simultaneously is a highly important but challenging issue in organic solar cells (OSCs). In this study, a benzotriazole-based p-type polymer (J61) and three benzotriazole-based nonfullerene small molecule acceptors (BTA1-3) are chosen to investigate the energetic driving force for the efficient charge transfer. The lowest unoccupied molecular orbital (LUMO) energy levels of small molecule acceptors can be fine-tuned by modifying the end-capping units, leading to high V-OC (1.15-1.30 V) of OSCs. Particularly, the LUMO energy level of BTA3 satisfies the criteria for efficient charge generation, which results in a high V-OC of 1.15 V, nearly 65% external quantum efficiency, and a high power conversion efficiency (PCE) of 8.25%. This is one of the highest V-OC in the high-performance OSCs reported to date. The results imply that it is promising to achieve both high J(SC) and V-OC to realize high PCE with the carefully designed nonfullerene acceptors.