To develop semiconductor detectors based on TlBr with excellent energy resolution at high yields, a variety of characterization methods for TlBr crystals are necessary. Among the various methods based on excitation by photons or ionizing radiation, we chose transient absorption measurements after the irradiation of pulsed electron beams to analyze the recombination dynamics of electron–hole pairs generated by the electron beams. The decay behavior of the transient absorption depended on the pulse intensity and was satisfactorily fitted with a decay function based on bimolecular recombination dynamics. The bimolecular recombination coefficients obtained from the fitting were similar for the samples cut from different parts of a crystal boule. Assuming that the recombination occurred through Shockley–Read–Hall bimolecular recombination via electronic levels of defects within the bandgap, the result indicates that the concentrations of the defects responsible for the recombination were similar for the samples out from different parts of the crystal boule.