The results of the studies of the orientational optical nonlinearity of a nematic host doped with high-molar-mass compounds of different molecular architecture such as a comb-like polymer and a dendrimer containing azobenzene chromophores are presented. The nonlinearity induced by these compounds was found to be higher than that induced by the low-molar-mass dyes similar in structure to the light-absorbing constituents of the polymer and dendrimer. Possible reasons for the nonlinearity enhancement for macromolecular dopants are discussed.