Hyperbranched structures of chromophores were developed to improve the nonlinearity of optical polymers. Macromolecules with 3-[p-(2'-hydroxyethylmethylamino)-styryl]-1-dicyanomethylene-5,5-dimethylcyclohex-2-ene (AIDC) were prepared using 3,5-dihydroxyphenyl groups as building blocks. When the molecule was incorporated into a polyimide backbone (PI-DAIDC101), a high electro-optic coefficient was obtained, giving 32 pm.V -1 at 1.55 μm. The nonlinearly is at least doubly enhanced in comparison with that of conventional side chain-optical polyimides. This is mainly attributable to an increased polarizing efficiency derived from the chromophore structures.