Temperature and frequency dependent 7 Li spin-lattice relaxation rate measurements on the layer-structured two-dimensional ion conductor Li x TiS 2 in different order states were carried out in the laboratory frame (T - 1 1 ) and in the rotating frame (T - 1 1 ). The activation energies for individual ion hopping, as obtained from these meauurements, are about 0.19 eV for the polycrystalline, 0.16 eV for the nanocrystalline, and 0.07 eV for the amorphous material. The frequency dependence of T - 1 1 is sublinear for both disordered modifications. The NMR central transition lines of the nanocrystalline material decompose into a narrow and a broad component in the course of motional narrowing. The relative intensity of the narrow component corresponding to the fraction of highly mobile Li ions increases gradually with temperature, reaching a limiting value of 50% at high temperatures. Hence, we conclude that the interfacial regions are not structurally homogeneous and comprise about half of the atoms of the sample. Contrary to three-dimensional nanocrystals, diffusion in the two-dimensional nanocrystalline material takes place on the grain surfaces rather than within an amorphous interface medium.