Cesium monocarba-hydroborate CsCB11H12 belongs to the family of alkali-metal closo- hydroborate salts which are considered as promising solid electrolytes for battery applications. To study the dynamical properties of this compound at the microscopic level, we have measured the 1H and 133Cs nuclear magnetic resonance (NMR) spectra and spin-lattice relaxation rates over the temperature range of 80–434 K. Our measurements have revealed a coexistence of two types of reorientational jump processes of the complex [CB11H12]− anions. For the faster of these processes characterized by the average activation energy of 310 meV, the anion reorientations are not “frozen” at the NMR frequency scale down to 120 K. The behavior of the 133Cs NMR line width in CsCB11H12 is consistent with the onset of long-range diffusive motion of Cs+ ions at the frequency scale of ∼104 s−1 above 340 K, and the distinct effects of the diffusive Cs+ jumps on both the 1H and 133Cs spin-lattice relaxation rates become observable above 380 K.