The first molecular hyperpolarizabilities (beta) of a series of 2,6-di-tert-butylindoanilines, measured by electric-field-induced second harmonic generation, are somewhat more sensitive to donor strength than was found for analogously substituted nitrostilbenes, and dimethylindoaniline has a beta roughly twice that of its 2,6 di-tert-butylated analogue, measured in chloroform; solvatochromic measurements on the former compound suggest that this decrease in hyperpolarizability is consistent with a bound-solvent effect.