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Abstract While the discovery of two-dimensional (2D) magnets opens the door for fundamental physics and next-generation spintronics, it is technically challenging to achieve the room-temperature ferromagnetic (FM) order in a way compatible with potential device applications. Here, we report the growth and properties of single- and few-layer CrTe 2 , a van der Waals (vdW) material, on bilayer graphene by molecular beam epitaxy (MBE). Intrinsic ferromagnetism with a Curie temperature ( T C ) up to 300 K, an atomic magnetic moment of ~0.21  $${\mu }_{{\rm{B}}}$$ μ B /Cr and perpendicular magnetic anisotropy (PMA) constant ( K u ) of 4.89 × 10 5  erg/cm 3 at room temperature in these few-monolayer films have been unambiguously evidenced by superconducting quantum interference device and X-ray magnetic circular dichroism. This intrinsic ferromagnetism has also been identified by the splitting of majority and minority band dispersions with ~0.2 eV at Г point using angle-resolved photoemission spectroscopy. The FM order is preserved with the film thickness down to a monolayer ( T C  ~ 200 K), benefiting from the strong PMA and weak interlayer coupling. The successful MBE growth of 2D FM CrTe 2 films with room-temperature ferromagnetism opens a new avenue for developing large-scale 2D magnet-based spintronics devices. 

Electric‐field‐controlled magnetism is of importance in realizing energy efficient, dense and fast information storage and processing. Strain‐mediated converse magneto‐electric (ME) coupling between ferromagnetic and ferroelectric heterostructure shows promise for realizing electric‐controlled magnetism at room temperature and is attracting a number of recent investigations. However, such ME‐effect studies have mainly focus on magnetic metals. In this work, high quality yttrium iron garnet (Y₃Fe₅O₁₂(YIG)) films are deposited directly onto (100)‐oriented single‐crystal Pb (Mg_1/3Nb_2/3)_0.7Ti_0.3O₃(PMN‐PT) substrates by means of magnetron sputtering. The electric‐field‐induced polarization switching and lattice strain in the PMN‐PT substrate results in two distinct magnetization states in the YIG film that are nonvolatile and electrically reversible. Because of the direct contact between the YIG and the PMN‐PT substrate, an efficient ME coupling and an almost 90° rotation of the easy axis of the YIG film can be realized. Furthermore, the electric‐field‐controlled hysteresis loop‐like ferromagnetic resonance field shifts and spin pumping signals are observed in Pt/YIG/PMN‐PT heterostructures. Thus, the obstacle is overcome via growing high‐quality YIG thin films directly onto PMN‐PT substrates and an efficient manipulation of magnetism and pure spin current transport by electric field is thereby realized. These findings are instructive for future low‐power magnetic insulator‐based spintronic devices.