Hundred-micrometer-sized calcium-aluminum-silicates (CAS) inclusions occur in moissanite-4H, moissanite-15R, and moissanite-6H from Turkey. These inclusions commonly consist of tabular exsolution lamellae of two different minerals. By combined electron microprobe and Raman spectroscopy analysis, at least eight different, essentially Mg- and Fe-free Ca-Al-silicate or Al-silicate phases have been discerned. The most common phase is dmisteinbergite, a hexagonal modification of CaAl2Si2O8, occurring in association with lamellae of Cax(Al,Si)1−xO3 or Ca1−x(Al,Si)2+xO5 compositions. All three phases contain significant amounts of BaO (up to 2 mol% of celsiane component in dmisteinbergite), SrO, SO3, and light rare earth elements (LREE). In particular, Ca1−x(Al,Si)2+xO5 contains up to 2.1 wt% of LREE, 3.9 wt% of F, and significant traces of Cl, while it is also associated to osbornite (TiN). Pure ghelenite, Ca2Al2SiO7, and three additional compositions, namely CaAl4−xSixO7, Ca1−x(Al,Si)3+xO6, and Ca3−x(Al,Si)6+xO14 have been found, either occurring as single grains or forming exsolution lamellae. They also contain significant amounts of BaO, SrO, SO3, and LREE. One last intriguing phase is composed in average of 65.9 wt% SiO2, 17.4% Al2O3, 3.0% alkalis, 6.0% BaO, 2.0% CaO+MgO, 0.9% ZrO2, and up to 0.5% LREE. Dmisteinbergite and ghelenite show Raman peaks in very good agreement with literature data, Cax(Al,Si)1−xO3 shows main Raman modes at 416 and 1009 cm−1, Ca1−x(Al,Si)3+xO6 at 531 and 1579 cm−1 while Ca3−x(Al,Si)6+xO14 has a strong peak at 553 cm−1. CaAl4−xSixO7 shows a weak Raman pattern, while Ca1−x(Al,Si)2+xO5 has no detectable Raman modes. Since the association moissanite-CAS is thermodynamically not stable at ambient pressure and moissanite crystals hosting the CAS phases have δ13C values typical of deep-mantle origin, we interpret the CAS inclusions as partially retrogressed HP minerals. Striking analogies exist between observed CAS compositions and experimentally obtained HP-HT mineralogy. For instance, Cax(Al,Si)1−xO3 contains up to 25 mol% of Al2O3, which is considered as the upper limit of alumina solubility in Ca-perovskite. The study confirms that CAS phases are an important mantle depository for large ion lithophile elements (LILE) and LREE.