2D room‐temperature magnetic materials are of great importance in future spintronic devices while only very few are reported. Herein, a plasma‐enhanced chemical vapor deposition approach is exploited to construct the 2D room‐temperature magnetic MnGa4‐H single crystal with a thickness down to 2.2 nm. The employment of H2 plasma makes hydrogen atoms can be easily inserted into the MnGa4 lattice to modulate the atomic distance and charge state, thereby ferrimagnetism can be achieved without destroying the structural configuration. The as‐obtained 2D MnGa4‐H crystal is high‐quality, air‐stable, and thermo‐stable, demonstrating robust and stable room‐temperature magnetism with a high Curie temperature above 620 K. This work enriches the 2D room‐temperature magnetic family and opens up the possibility for the development of spintronic devices based on 2D magnetic alloys.
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