Control of the shape and structure of nanoscale objects and the nanoengineering of noncentrosymmetric macroscopic material lattices has been used to achieve record electro-optic activity. Multi-chromophore-containing dendrimer structures have been designed to optimize molecular hyperpolarizability and to control intermolecular electrostatic interactions that dominate the macroscopic organization of dendrimers. New condensed matter theory, that explicitly takes into account long-range, spatially-anisotropic intermolecular electrostatic interactions among large numbers of high dipole moment chromophores, has been developed and used to design nanoscale objects ideally suited to be assembled into noncentrosymmetric lattices by techniques such as electric field poling. This new theory permits quantitative investigation of crystallization and phase-separation phenomena. Organic materials exhibiting electro-optic coefficients in excess of 100 pm/V at telecommunication wavelengths have been fabricated. The time response of these materials to applied electric fields is defined by the pi-electron structure of the materials and is on the order of femtoseconds. These materials permit fabrication of electro-optic devices characterized by operational bandwidths of greater than 100 GHz and drive voltage requirements of less than 1 volt. Moreover, organic electro-optic materials permit fabrication of sophisticated 3-dimensional active/passive optical circuitry and integration with both VLSI semiconductor electronics and silica fiber optics. New organic electro-optic materials are widely applicable to telecommunications (both satellite and fiber optic), information processing, transportation, display, sensing, and defense industries. Among prototype devices fabricated from these materials, exhibiting never-before-achieved performance, are included integrated (chip scale) WDM transmitter-receivers, phased array radars, ultrafast analog-to-digital converters, optical switches, large angle spatial light modulators, ultrahigh bandwidth and ultrastable oscillators, ultrahigh bandwidth spectrum analyzers, ultrahigh bandwidth low drive voltage electrical-to-optical signal transducers, optical gyroscopes, and broadband detectors (including terahertz signal generators and detectors). In some cases, performance of nanostructured organic electro-optic materials has been improved by integrating these materials into photonic bandgap and ring microresonator architectures.