For Li3InCl6, we find two distinct motional processes where one of the processes appears to dominate the long range diffusion and transport. From the layered structure, the diffusion path analysis and consideration of the most likely jump events, we assign the fast diffusion jump process to jumps within the Li layer in the ab-plane, and the slower jump process to jumps along the c-direction. Upon Zr substitution, the path along the c-direction seems to open up, due to a reduction in the In occupancy on the mixed In2/Li4 site. The second jump process probed for the pristine sample disappears for the substituted versions, and they most likely approach the timescale of the first, indicating reduced anisotropy. Nevertheless, the NMR spectral density fitting did not lead to an unambiguous choice of a spectral density. The residual chemical shift anisotropy in the static lineshapes of the substituted materials is less than that observed for the pristine material, though it is not completely averaged out. While the reduction could be due to a larger distribution in local environments due to the introduction of Zr, the fact that there is residual chemical shift anisotropy indicates that also for the substituted materials, the motion does not include all sites equally, even on longer timescales, and is hence anisotropic. intensities, which were assumed to be due to preferential orientation. Therefore, the powder was ball-milled, to reduce the crystallite size. The ball-milled powder, however, had an order of magnitude lower ionic conductivity, and showed very broad peaks in the x-ray diffraction pattern. Therefore, the fine powder was annealed again, which gave the desired combination of high ionic conductivity, but an x-ray diffraction pattern of sufficient quality for Rietveld refinement. Recent research suggests that materials of the here investigated Li3MX6 structure families exhibit varying degrees of stacking faults . It can't be excluded that the reason for the varying intensities here are due to a different peak shape due to possible stacking faults, but in the final synthesis product stacking faults were not needed for the final Rietveld refinement.