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We review recent transformative advances in materials design, synthesis, and processing as well as device engineering for the utilization of organic materials in hybrid electro-optic (EO) and optical rectification (OR) technologies relevant to telecommunications, sensing, and computing. End-to-end (from molecules to systems) modeling methods utilizing multi-scale computation and theory permit prediction of the performance of novel materials in nanoscale device architectures including those involving plasmonic phenomena and architectures in which interfacial effects play a dominant role. Both EO and OR phenomenon require acentric organization of constituent active molecules. The incumbent methodology for achieving such organization is electric field poling, where chromophore shape, dipole moment, and conformational flexibility play dominant roles. Optimized chromophore design and control of the poling process has already led to record-setting advances in electro-optic performance, e.g., voltage-length performance of < 50 volt-micrometer, bandwidths > 500 GHz, and energy efficiency < 70 attojoule/bit. They have also led to increased thermal stability, low insertion loss and high signal quality (BER and SFDR). However, the limits of poling in the smallest nanophotonic devices—in which extraordinary optical field densities can be achieved—has stimulated development of alternatives based on covalent coupling of modern high-performance chromophores into ordered nanostructures. Covalent coupling enables higher performance, greater scalability, and greater stability and is especially suited for the latest nanoscale architectures. Recent developments in materials also facilitate a new technology—transparent photodetection based on optical rectification. OR does not involve electronic excitation, as is the case with conventional photodiodes, and as such represents a novel detection mechanism with a greatly reduced noise floor. OR already dominates at THz frequencies and recent advances will enable superior performance at GHz frequencies as well.