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A new two-photon absorption compound, 2-{4-[(dicyanomethylidene-5,5-dimethylcyclohexl)vinyl]phenyl}imidazo[4,5-f][1,10]phenanthroline (DDVPIP), was synthesized and characterized. The one-photon excited fluorescence (OPRF) and two-photon excited fluorescence (TPEF) of DDVPIP are sensitive to the acid/base of the solution, which are enhanced in basic solution but weakened in acidic solution. Charge-transfer (CT) states of DDVPIP were calculated through theory methods to explain its acid/ base-sensitive fluorescent properties.