The layered fast ion conductor LixTiS2 (x approximate to 2/3) has been prepared in nanocrystalline (n-LixTiS2) and amorphous (a-LixTiS2) forms. Hence, a direct comparison of the lithium diffusion in a homogeneously and a heterogeneously disordered material with the-same composition is possible. As a reference system, polycrystalline LixTiS2 (in its hexagonal modification, h-LixTiS2) was also investigated by measuring the temperature and frequency dependencies of the spin-lattice relaxation rate T-1(-1) of Li-7. The activation energies for individually jumping ions as obtained from the low-temperature flanks of the rate maxima are 190, 160, and 70 meV in h-,n-, and a-LixTiS2, respectively. The frequency dependence of T-1 is sublinear for both disordered forms, which is explained in terms of the unified site relaxation model. Li-7 nuclear magnetic resonance (NMR) spectra of n-LixTiS2 tend, contrary to those of h-LixTiS2 and a-LixTiS2, to decompose into broad and narrow central line components. The relative intensity of the narrow component, which is attributed to fast moving Li ions in the interfacial regions, is temperature dependent and reaches 50% at 360K. A schematic model for the ionic conduction process in two-dimensional nanocrystalline fast ionic conductors Is proposed, introducing grain surface pathways as the dominant track for mobile ions.