Terbium-exchanged ultrastable Y (USY) zeolites were investigated by using time-resolved photoluminescence spectroscopy techniques and methods. To determine the distribution of terbium species in USY zeolites together with their photoluminescence properties, several analysis methods for the time-resolved luminescence spectra were used such as the area normalization of time-resolved photoluminescence spectra, singular value decomposition, global nonlinear least squares, and the maximum entropy. Except for a questionable long lifetime, small contribution of a terbium species with lifetime of 1.9–2.1 ms, all the experimental and analysis results converged to a two terbium species distribution with lifetimes varying between 410–440 and 1000–1100 μs. The effects of the silylation of terbium-exchanged USY zeolites with phenyl-, vinyl-, and hexadecyltrimethoxysilanes on the lanthanide’s photoluminescence properties were also described.