Searching for layered MAX phase-like materials with properties of both ceramics and metals is a topic in its infancy. Herein, through a combination of crystal structure, electronic structure, chemical bonding, and elastic property investigations, we report two MAX phase-like layered materials Rh 2 YSi and Ir 2 YSi. ties that they display. 5,6,9,10 These layered structure materials can also be used as precursors or parent materials for producing two-dimensional materials such as graphenebased (GB) and graphene-like (GL) materials 11 through mechanical exfoliation (micromechanical cleavage) or chemical approaches. MAX phases, a family of layered ternary carbides and nitrides with a general formulae of M n+1 AX n (where M is an early transition metal, X is carbon or nitrogen, A is III A , IV A , V A , or VI A group elements, n = 1, 2, 3, 4, 5, and 6), are typical layered materials which exhibit a unique combination of both ceramic-like and metallic properties. 5,[12][13][14][15][16][17][18][19] For example, like ceramics, they have low density, high strength and modulus, good corrosion, and high-temperature oxidation resistance 20 ; like metals, they are electrical conductive, relatively soft and readily machinable, resistant to thermal shock, and tolerant to damage.