Efficient exciton dissociation is crucial to obtaining high photonic response in photodetectors. This work explores implementation of a novel exciton dissociation mechanism through heterojunctions self-assembled at the graphene/MWCNT (multiwall carbon nanotube) interfaces in graphene/MWCNT nanohybrids. Significantly enhanced near-infrared photoresponsivity by nearly an order of magnitude has been achieved on the graphene/MWCNT nanohybrids as compared to the best achieved so far on carbon nanotube (CNT) only infrared (IR) detectors. This leads to a high detectivity up to 1.5 × 10(7) cm·Hz(1/2)·W(-1) in the graphene/MWCNT nanohybrid, which represents a 500% improvement over the best D* achieved on MWCNT film IR detectors and may be further improved with optimization on the interfacial heterojunctions. This approach of the self-assembly of graphene/CNT nanohybrids provides a pathway toward high-performance and low-cost carbon nanostructure IR detectors.