Abstract High-performance quantum anomalous Hall (QAH) systems are the crucial materials to explore emerging quantum physics and magnetic topological phenomena. Inspired by layered FeSe materials with excellent superconducting properties, the Janus monolayers Fe2SSeX2 (X = Ga, In, and Tl) are built by the decoration of Ga, In, and Tl atoms in monolayer Fe2SSe. Using the first-principles calculations, the Fe2SSeX2 have stable structures and prefer ferromagnetic (FM) orders, which belong to the Weyl semimetal without spin-orbit coupling (SOC). For the out-of-plane (OOP) magnetic anisotropy, the large nontrivial gaps are opened, and the Fe2SSeX2 are predicted to be large-gap QAH insulators with high Chern-number C = 2, proved by two chiral edge states and Berry curvatures. When the magnetization is flipped, two chiral edge states can be simultaneously changed and C = -2 can be obtained, revealing one fascinating behavior of chiral spin-edge-state locking. It is found that the QAH properties of the Fe2SSeX2 are robust against the strain. Especially, the nontrivial topological quantum states can spontaneously appear for the Fe2SSeGa2 and Fe2SSeIn2, because the easy magnetic axis orientations are adjusted from in-plane to OOP by the biaxial strain. Our studies provide excellent candidate systems to realize the QAH properties with high Chern-number, and advocate more experimental explorations in the combination of superconductivity and topology.
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