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Third-order optical nonlinearities of silicon 2,3-naphthalocyanine bis(trihexylsilyloxide) (SiNc) were measured by femtosecond degenerate four-wave mixing technique under resonant conditions. The time dependence of the signals indicates that the electronic response dominates the mechanism. The electronic molecular hyperpolarizability γe of SiNc was determined to be as high as 2 × 10-28 esu, which is the largest value reported so far to our knowledge. The electronic third-order susceptibility for a pure SiNc film has been measured to be 4 × 10-7 esu.The large nonlinear susceptibility was discussed in terms of J-type molecular arrangement.