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Wastewater containing low concentrations of rare earth ions not only constitutes a waste of rare earth resources but also threatens the surrounding environment. It is therefore necessary to develop environmentally friendly methods of recovering rare earth ions. The spores produced by Bacillus are resistant to extreme environments and are effective in the bioadsorption of rare earth ions, but their adsorption behaviors and mechanisms are not well understood. In this study, the cells and spores of Bacillus subtilis PS533 and PS4150 were used as biosorbents, and their adsorption of terbium ions was compared under different conditions. The adsorption characteristics of the spores were investigated, as were the possible mechanisms of interaction between the spores and rare earth ions. The results showed that the PS4150 spores had the best adsorption effect on Tb(III), with the removal percentage reaching 95.2%. Based on a computational simulation, SEM observation, XRD, XPS, and FTIR analyses, it was suggested that the adsorption of Tb(III) by the spores conforms to the pseudo−second−order kinetics and the Langmuir adsorption isotherm model. This indicates that the adsorption process mainly consists of chemical adsorption, and that groups such as amino, hydroxyl, methyl, and phosphate, which are found on the surface of the spores, are involved in the bioadsorption process. All of these findings suggest that Bacillus subtilis spores can be used as a potential biosorbent for the recovery of rare earth ions from wastewater.