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In 2017, we discovered quaternary i-MAX phases-atomically layered solids, where M is an early transition metal, A is an A group element, and X is C-with a (M 1 2/3 M 2 1/3)2AC chemistry, where the M 1 and M 2 atoms are in-plane ordered. Herein we report on the discovery of a class of magnetic i-MAX phases in which bi-layers of a quasi-2D magnetic frustrated triangular lattice overlays a Mo honeycomb arrangement and an Al Kagomé lattice. The chemistry of this family is (Mo2/3RE1/3)2AlC, and the rare earth elements, RE, are Ce, Pr, Nd, Sm, Gd, Tb, Dy, Ho, Er, Tm, and Lu. The magnetic properties were characterized and found to display a plethora of ground states, resulting from an interplay of competing magnetic interactions in the presence of magnetocrystalline anisotropy. This material is available free of charge via the Internet at http://pubs.acs.org.

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