The fluorescent characteristics of Troger's base have been investigated experimentally. A one-photon-induced fluorescent spectrum was observed, and the peak wavelength was at 337 nm with a full width at half-maximum of ~85nm . The violet radiation of the Troger's base crystal could result from the pi(*) -pi transition of the benzenoid pi bond. Two-photon-pumped frequency-upconverted fluorescence was obtained, which is a wideband emission with the main peak wavelength at 337 nm and a subordinate peak. Donor groups and acceptor groups of electrons in the aromatic rings strengthen the two-photon-pumped frequency-upconverted fluorescence.