摘要： Monolayer transition-metal dichalcogenides have inspired worldwide efforts in optoelectronic devices but real applications are hindered with their reduced optical absorption due to their atomically ultrathin signature. In this study, by utilizing their biradical nature such as excellent absorption coefficient, broad bandwidth from the ultraviolet to near-infrared region, and small triplet–singlet energy gap, a series of helicene 5,14-diaryldiindeno[2,1-f:1′,2′-j]picene (DDP) derivatives (1ab, 1ac, and 1bb) are integrated with monolayer MoS2 for extraordinary photodetector performance and outstanding stability. Via comprehensive time-resolved studies, the interfacial charge-transfer process from the DDPs to the MoS2 layer is evidenced by the stabilized exciton property of the organics (1ac)/MoS2 heterostructure. Significantly, the 1ac/MoS2 photodetector exhibits an ultrahigh photoresponsivity of 5 × 107 A W?1 and a fast response speed of 45 ms due to the highly efficient photoexcited carrier separation and the matched type-II energy band alignment. The biradical 1ac/MoS2 hybrid photodetector shows no sign of degradation after one-month operation. The results pave a new avenue for biradical based high-performance and super-broadband optoelectronic devices.