Reutilization of industrial waste products as cement additives yields a number of secondary materials, yet their identification is not always trivial. Confirmation of the formation of a LDH-type (phyllosilicate/carbonate) material is the main purpose of this study. Mineralogically, organic and inorganic compounds form some industrial wastes, among which the phyllosilicates are prominent. Crystalline and amorphous hydrated phases appeared during the pozzolanic reaction in a dehydroxylated phyllosilicate/lime system, whose controlled activation yielded dehydroxylated products with high pozzolanic properties. The LDH-type (phyllosilicate/carbonate) material was one of the reaction products; this material could be considered as the superposition type 1:1 of tetrahedral layers of silicon and aluminum and octahedral layers of aluminum (dehydroxylated kaolinite), generating a positive charge in the interlaminar region compensated by carbonate anions with a basal spacing (001) measured by XRD at 7.57Å. Therefore, several techniques were used to determine whether they could be included in the structural group named Layered Double Hydroxides (LDHs), as they are, too, laminar layers of oxides and hydroxides with a positive laminar charge in the interlayer region compensated by the presence of anions with similar basal spacing. In this research, the effects of activation temperature and calcite proportion were analyzed on the hydrated phases formed after 28 days of pozzolanic reaction in a metakaolin (MK)/lime system. The MK was obtained from a mix of 1:1; 2:1 and 3:1 kaolinite:calcite mixture, thermally activated at 750°C for 2 hours, comparing it with kaolinite activated at 600°C for 2 hours. As the most LDH-rich sample, the 1:1 LDH-type (phyllosilicate/carbonate) phase was characterized using XRD, SEM-EDX, HRTEM-EDX, FTIR, NMR-MAS, and Raman spectroscopy. K E Y W O R D S calcium silicate hydrate, LDH type (phyllosilicate carbonate), metakaolin, Portland cement, SEM, transmission electron microscopy, X-ray diffraction | 4991 SÁNCHEZ Et al. How to cite this article: Sánchez I, Ramírez M, Casas Angulo M, et al. Characterization of LDH (phyllosilicate/carbonate) type compounds formed in the pozzolanic reaction of phyllosilicate-rich industrial waste. J Am Ceram Soc. 2019;102:4990-4998. https://