In order to fully characterize crystal aggregates, the orientation of primary particles has to be analyzed. A procedure for extracting this information from three-dimensional microcomputed tomography (lCT) images was recently published by our group. We here extend this method for asymmetrical crystals and apply it for studying the disorientation angle distribution of four potash alum crystal samples that were obtained under various experimental conditions. The results show that for all considered supersaturation profiles, primary particle pairs tend to have the same orientation significantly more often than in theoretical considerations, in which the orientations of primary particles are assumed to be distributed randomly. (C) 2017 Elsevier B.V. All rights reserved.