A MoSiBEA zeolite has been prepared by a two-step postsynthesis procedure that consists of first creating the vacant T-atom sites with associated silanol groups by treatment of TEABEA zeolite with nitric acid and then incorporating Mo ions into the vacant T-atom sites by solid-state ion exchange at 773 K using molybdenum(II) acetate. The incorporation of Mo ions into the vacant T-atom sites of the framework of SiBEA zeolite as isolated mononuclear Mo(VI) species was evidenced by the combined use of XRD and FTIR, NMR, and diffuse reflectance UV-visible spectroscopies. The consumption of OH groups was monitored by FTIR spectroscopy. The reducibility of Mo was investigated by TPR and EPR spectroscopy. The size of very small well-dispersed Mo(0) nanoparticles formed upon treatment of MoSiBEA between 298 and 1240 K in hydrogen stream (5% H2/Ar) was measured by TEM.