Spin-lattice relaxation rates (T-1(-1)) for Li-7 and Cs-133 nuclear magnetic resonance in the nonlinear optical crystal CsLiB6O10 were measured in the temperature range 20-300 K. The dominant relaxation of this crystal in the whole temperature investigated is due to quadrupolar interaction. Li-7 spin-lattice relaxation time on the CsLiB6O10 yielded a minimum, attributed to the effect of molecular motion. These experiments have been analyzed by BPP theory, and the activation energy for the molecular motion was determined to be 21.19 kJ/mol. T-1(-1) for the Cs-133 nucleus is well described with the simple power law of T-1(-1) = AT(k) + B, where T is the temperature. The measured relaxation rate was found to be proportional to the T-2. The temperature dependence of the relaxation rates for the Cs-133 nucleus in a CsLiB6O10 single crystal is in accordance with a Raman process. (C) 2002 Elsevier Science Ltd. All rights reserved.