Jin, CuiShang, JingTang, XiaoTan, XinSmith, SeanNiu, ChengwangDai, YingKou, Liangzhi2022-05-092050-7526http://hdl.handle.net/1885/264617A 2D FeTiO3 magnetic monolayer which was recently exfoliated from non-van der Waals layered bulk crystals has opened the research era of low-dimensional magnets, however its structural and chemical instability hampered its practical application. Through first-principles calculations, we found that the stability of 2D FeTiO3 can be obviously enhanced by a monolayer Ti2CO2 substrate and simultaneously the magnetic/electronic properties can be well regulated. Depending on the FeTiO3/Ti2CO2 stacking configurations, the system exhibits different magnetic and electronic behaviors, which can be either ferromagnetic or antiferromagnetic with the feature of half-metallic (with 100% spin-polarization ratio) or metallic. Moreover, it was also found that the interfacial magnetic coupling orders can be precisely modulated with an external electric field (0.4 to 0.2 V Å1 ). In particular, the Curie temperature is predicted to be 315 K, rendering the magnetism stable at room temperature. These interesting properties make 2D FeTiO3/Ti2CO2 a promising candidate material for spintronic device applications.C. J. gratefully acknowledges financial support from the China Scholarship Council (CSC, 201706220175). L. K. gratefully acknowledges financial support from the ARC Discovery Project (DP190101607)application/pdfen-AUThis journal is © The Royal Society of Chemistry 2019201910.1039/c9tc04979g2022-06-12