AbstractThree kaolinite reference samples identified as KGa-1, KGa-1b, and KGa-2 from the Source Clays Repository of The Clay Mineral Society (CMS) are used widely in diverse fields, but the defect structures have still not been determined with certainty. To solve this problem, powder diffraction patterns of the KGa-1, KGa-1b, and KGa-2 samples were modeled. In a kaolinite layer among three symmetrically independent octahedral sites named as A, B, and C and separated from each other by b/3 along the b parameter, the A and B sites are occupied by Al cations, whereas, the C sites located along the long diagonal of the oblique kaolinite unit cell are vacant. The layer displacement vectors t1 and t2 are related by a pseudo-mirror plane from defect-free 1Tc kaolinite enantiomorphs, whereas, the random interstratification within individual kaolinite crystallites creates right-hand and left-hand layer sub-sequences producing structural disorder. A third layer displacement vector, t0, located along the long diagonal of the oblique layer unit cell that contains the vacant octahedral site and coincides with the layer pseudo-mirror plane may exist. Thus, a structural model should be defined by the probability of t1, t2, and t0 layer displacement translations Wt1, Wt2, and Wt0, respectively, determined by simulated experimental X-ray diffraction (XRD) patterns. X-ray diffraction patterns were calculated for structures with a given content of randomly interstratified displacement vectors, and other XRD patterns were calculated for a physical mixture of crystallites having contrasting structural order with only C-vacant layers. The samples differ from each other by the content of high- and low-ordered phases referred to as HOK and LOK. The HOK phase has an almost defect-free structure in which 97% of the layer pairs are related by just the layer displacement vector t1 and only 3% of the layer pairs form the enantiomorphic fragments. In contrast, the LOK phases in the KGa-1, KGa-1b, and KGa-2 samples differ from HOK phases by the occurrence probabilities for the t1, t2, and t0 layer displacements. In addition, the LOK phases contain stacking faults that displace adjacent layers in arbitrary lengths and directions. Low XRD profile factors (Rp = 8-11%) support the defect structure models. Additional structural defects and previously published models are discussed.