Near‐infrared organic photodetector (NIR OPD) is promising for emerging wearable biosensing applications. However, their practical application is hindered by the high dark currents of devices that limit the detection of faint light. In this work, highly sensitive flexible NIR OPDs are presented with ultralow dark currents, fabricated using a layer‐by‐layer blade coating (LBL‐BC) technique. In the active layer, a fully fused‐ring molecule FM2, featuring a fixed molecular skeleton, is employed as an electron acceptor to reduce the trap density. The LBL‐BC method enhances the film order and phase purity of the active layer, significantly reduces the trap density of states, and optimizes the vertical phase separation structure of the thin film, thereby preventing reverse charge injection. As a result, a highly sensitive flexible NIR OPD is developed exhibiting an ultralow dark current density of 4.83 × 10−9 A cm−2 at −0.3 V bias and an extremely low noise current density of 7.65 × 10−15 A Hz−1/2 at 10 Hz, comparable to commercial silicon photodiodes. Furthermore, this flexible device is successfully applied for real‐time monitoring of human heartbeat rate, oxygen saturation, and motion recognition. These findings advance the development of highly sensitive NIR OPDs and their application in wearable biosensing technologies.