Measurements of the C-13, Li-7, and H-1 nuclear magnetic resonance (NMR) of the nanocomposite formed by the intercalation of lithium and diethylamine in molybdenum disulfide, Li0.1MoS2[(C2H5)(2)NH](0.2), are reported. The strong Li-Li dipolar interaction strength, calculated from the Li-7 NMR decoupling data, suggests the formation of lithium clusters. The dimensional restriction of the available space between the host layers supports a hypothesis that is based on the formation of Li-3 clusters stabilized by amine ligands. The lithium relaxation is mainly due to the interaction between the quadrupolar moment of the Li-7 nuclei and the fluctuating electric field gradient at the site of the nucleus, produced by the surrounding charge distribution. The dynamical parameters obtained from the Li-7 temperature dependence of the spin-lattice relaxation indicate a high lithium mobility, which is attributed to the fast exchange motion of the lithium ions between the coordination sites within each Li-3 aggregate. The H-1 line shape and relaxation data support the proposed structural model for the lithium-diethylamine cluster. Numerical analysis of the H-1 line shape indicates that the intercluster dipole-dipole interactions are responsible for most of the spectral broadening. H-1 spin-lattice relaxation is mainly governed by hydrogen nuclei in the less-mobile CH2 and in the fast-relaxing CH3 groups in the diethylamine molecule.