Major Goals Carbon-based nanostructures including nanotubes CNTs and graphene have superior electronic, optoelectronic and mechanical properties, which provide tremendous opportunities for design of novel optoelectronic devices of extraordinary performance in addition to the benefits of low cost, large abundance, and light weight. Our recent demonstrations of uncooled infrared detectivity D of 3.4x109 cmHz12W on individual multiwall CNT infrared detectors with asymmetric Schottky contacts, D of 2.3x108 cmHz12W in a photoconductor based on semiconductive singe-wall CNTs and conjugated semiconductor Poly3-hexylthiophene polymer s-SWCNTP3HT nanohybrid thin films, photoconductive gain up to 108 at zero VBG together with fast photoresponse on graphene field effect transistor with GaSe-nanosheets sensitizer, and responsivity 1.62 AWV on the ZnO nanowiregraphene hybrid ultraviolet detectors, highlight a few examples developed under our prior ARO support and illustrate fresh opportunities in exploration of nanohybrids between carbon nanostructures and other functional materials targeting at unprecedented physical properties demanded for high-performance photodetection. The proposed research builds upon the discoveries made through our prior ARO project, but aims to take it to the next level of high-performance photonic devices through atomistic interface design of exciton dissociation and charge transfer at the interfaces of nanohybrids through a thorough understanding of the fundamental physics governing the optoelectronic behaviors. Besides high performance and low cost, the proposed nanohybrid approach also has the advantage in its compatibility with Si-based readout circuits with micronanofabrication schemes employed for scaling up the proposed devices. Technology transfer for commercialization will be an emphasis of the proposed research.