Chromophores composed of 4-cyano-5-dicyanomethylene-2-oxo-3-pyrroline (CDCOP) and a donor have been synthsized for electrooptic applications. Three substituents of [5-(4-aminophenyl)-2-thienyl]-substituted CDCOP 1 and (4-aminophenyl)-substituted CDCOP 2 were modified to suppress the aggregation for effective poling. To 1, bulky and branched 2-ethylhexyl groups were introduced instead of linear alkyl groups. Less aggregation was confirmed in the polymer dispersion films, and the corona poling behaviors were examined. To 2, we introduced norbornyl epoxide groups as bulky and thermally crosslinkable moieties. The aggregation was suppressed as well, and the thermal crosslinking of the epoxide with acid anhydride in the presence of a base was investigated.