The process of particle aggregation significantly affects ash settling dynamics associated with volcanic explosive eruptions. Several experiments have been carried out to investigate the physics of ash aggregation and dedicated numerical schemes have been developed to produce more accurate forecasting of ash dispersal and sedimentation. However, numerical description of particle aggregation is complicated by the lack of complete datasets on natural samples required for model validation and calibration. Here we present a first comprehensive dataset for the internal structure, aerodynamical properties (e.g., size, density, terminal velocity) and grain size of constituting particles of a variety of aggregate types collected in the natural laboratory of Sakurajima Volcano (Japan). Even though the described particle clusters represent the most common types of aggregates associated with ash-rich fallouts, they are of difficult characterization due to the very low potential of preservation in tephra-fallout deposits. Properties were, therefore, derived based on a combination of high-resolution-high-speed videos of tephra fallout, scanning electron microscope analysis of aggregates collected on adhesive paper and analysis of tephra samples collected in dedicated trays. Three main types of particle clusters were recognized and quantitively characterized: cored clusters (PC3), coated particles (PC2), and ash clusters (PC1) (in order of abundance). A wide range of terminal velocities (0.5–4 m/s) has been observed for these aggregates, with most values varying between 1 and 2 m/s, while aggregate size varies between 200 and 1,200 µm. PC1, PC2, and PC3 have densities between 250 and 500, 1,500 and 2,000, and 500 and 1,500 kg/m3, respectively. The size of the aggregate core, where present, varies between 200 and 750 µm and increases with aggregate size. Grain size of tephra samples was deconvoluted into a fine and a coarse Gaussian subpopulation, well correlated with the grain size of shells and of the internal cores of aggregates, respectively. This aspect, together with the revealed abundance of PC3 aggregates, reconciles the presence of a large amount of fine ash (aggregate shells) with coarse ash (aggregate cores) and better explains the grain size distribution bimodality, the high settling velocity with respect to typical PC1 velocities and the low settling velocities of large aggregates with respect to typical PC2 velocity. Furthermore, ash forming the aggregates was shown to be always finer than 45 µm, confirming the key role played by aggregation processes in fine ash deposition at Sakurajima.