A family of new polymeric nonlinear optical materials with high second order non-linearities, good thermo-oxidative and reorientational stability, and low waveguide losses have been prepared from a series of chromophores containing hydrazone moieties. These new polymerizable chromophores can be readily prepared by the acid-catalyzed condensation of substituted arylhydrazines with functionalized ketones or aldehydes to give molecules that have μ3 values up to 2440 × 10−48 esu (1579 nm) in solution. Thermoplastic polycarbonates and poly(hydroxy ethers) containing hydrazone chromophores have been prepared with Tg's ranging from 135 °C to 285 °C. Epoxy systems crosslinked with amino-functional arylhydrazones, have high d33 values and high glass transition temperatures, albeit with lower relative thermo-oxidative stability. Simple Mach-Zehnder modulators and registered multi-level structures based on these polymers have been reported previously. One device, prepared from a hydrazone-containing poly(hydroxy ether), has an r33 value of 10 pm/V (1320 nm), and retains most of that activity to 140 °C.