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The Al4Ba crystal structure is the most common structure among binary intermetallic compounds. It is well suited for accommodating large atoms of group II elements and is often the intermediate phase closest to the terminal phase. It is, therefore, of interest to characterize diffusion properties of compounds with this tetragonal crystal structure. In the present study, 111In perturbed angular correlation spectroscopy was used to study solute site occupation and atom movement in In4Ba, Al4Ba, Al4Eu, Al4Sr, and Ga4Sr. The indium tracer and its daughter cadmium were found to occupy only the two Al-type sublattices in these compounds through detection of nuclear quadrupole interactions with axially symmetric EFGs. Measurements with increasing temperature revealed merging of signals due to dynamical averaging of these interactions as Cd atoms jumped at increasing rates between alternating sublattices. The jump rates were estimated to be between 8 kHz and 2 MHz at about 350 °C for Al4Eu and at about 450 °C for In4Ba and Al4Ba. Fits of spectra using Blume’s stochastic model allowed determination of activation enthalpies for average Cd jump rates between alternating Al sublattices in Al4Sr and Ga4Sr to be 1.16(3) eV and 1.47(3) eV, respectively. This result was used to estimate transverse diffusivities of Cd.