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Third-order optical nonlinearities and dynamic responses of two imino squaramides under neutral and base conditions were studied using the femtosecond degenerate four-wave mixing technique at 800nm.Ultrafast optical responses have been observed and the magnitude of the second-order hyperpolarizabilities of the squaramides has been measured to be as large as 10 31 esu. The absorption spectra,color of solution,and third-order optical nonlinearities of two imino squaramides change with the addition of sodium hydroxide.The γ value under the base condition for each dye is approximately 1.25 times larger than that under neutral conditions.