Three novel conjugated polymers with N-arylpyrrole as the conjugated bridge were designed and synthesized, which emitted strong one-or two-photon excitation fluorescence in dilute tetrahydrofuran (THF) solution with high quantum yields. The maximal two-photon absorption (TPA) cross-sections of the polymers, measured by the two-photon-induced fluorescence method using femtosecond laser pulses in THF, were 752, 1114, and 1869 GM, respectively, indicating that the insertion of electron-donating or electron-withdrawing moieties into the polymer backbone could benefit to the increase of the TPA cross-section. Their large TPA cross-sections, coupled with the relatively high emission quantum yields, made these conjugated polymers attractive for practical applications, especially two-photon excited fluorescence. (C) 2011 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 49: 2538-2545, 2011