Experimental investigations in a recirculating wind tunnel of the mechanisms of formation of accretionary lapilli have demonstrated that growth is controlled by collision of liquid-coated particles, due to differences in fall velocities, and binding as a result of surface tension forces and secondary mineral growth. The liquids present on particle surfaces in eruption plumes are acid solutions stable at 100% relative humidity, from which secondary minerals, e.g. calcium sulphate and sodium chloride, precipitate prior to impact of accretionary lapilli with the ground. Concentric grain-size zones within accretionary lapilli build up due to differences in the supply of particular particle sizes during aggregate growth. Accretionary lapilli do not evolve by scavenging of particles by liquid drops followed by evaporation — a process which, in wind tunnel experiments, generates horizontally layered hemispherical aggregates. Size analysis of particles in the wind tunnel air stream and particles adhering to growing aggregates demonstrate that the aggregation coefficient is highly grain-size dependent. Theoretical simulation of accretionary lapilli growth in eruption plumes predicts maximum sizes in the range 0.7–20 mm for ash cloud thicknesses of 0.5–10 km respectively