Fe- and Al-rich metapelite from the Transangarian segment of the Yenisey Ridge (East Siberia, Russia) is a potential new source of high-alumina refractories. The rocks have relatively high average contents of Al2O3 (20 wt%) and Fe2O3 (7.91 wt%), moderate K2O (3.44 wt%), and low CaO (0.74 wt%). Their dominant mineral assemblages are andalusite + muscovite + margarite + chlorite + biotite + quartz or staurolite + kyanite or/and andalusite + chlorite + muscovite + biotite + quartz with ±garnet and ±plagioclase. Al2SiO5 polymorphs occur as up to 1.5 cm andalusite porphyroblasts and partial or complete pseudomorphs after andalusite (kyanite and staurolite). Accessories include abundant Fe–Ti oxides and sporadic REE-, Y-, Ca-phosphates; sulfides are negligible. The composition of Al2SiO5 concentrates obtained in laboratory by heavy-media and magnetic separation from ≥0.06 mm fractions meet all requirements for raw material of this type: >56 wt% Al2O3, <42 wt% SiO2, <1 wt% Fe2O3, <1.2 wt% TiO2, and <0.2 wt% (CaO + MgO). The andalusite, kyanite, and mixed ores yield 0.7–4.1 wt%, 0.7–2.2 wt%, and 1.9–6.0 wt% of concentrate, respectively. The best-quality ores rich in Al2SiO5 polymorphs reside in zones of contact and/or dynamic metamorphism superimposed over regional metamorphism of Al-rich rocks.