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New symmetrical pi‐conjugated molecules having large third‐order nonlinear susceptibilities, χ(3), are reported. The χ(3) spectra of these molecules have been measured by a THG Maker‐fringe method. The magnitudes of the three‐photon resonant χ(3) reach 10-10 esu. The positions of the three‐photon resonance lie at the lowest‐energy peaks in the vibrational structure of each absorption spectra for these molecules.