coupling in multiferroics has attracted considerable research interests due to the wide range of applications in high-density information storages and low-energyconsumption spintronic devices. [7][8][9][10][11][12][13][14] Notably, the manipulation of magnetism by electric field has shown the transformative potential in the next-generation logic devices. [15][16][17][18][19][20][21][22][23][24] Nevertheless, the magnetoelectric coupling is extremely weak in traditional type-I multiferroics because of the mutually exclusive origins between ferroelectricity and ferromagnetism. In this context, searching for new types of multiferroics, especially at 2D community, is of great significance.Monolayer Hf 2 VC 2 F 2 was predicted to be a type-II multiferroic with a high phase transition temperature. [25] The ferroelectric polarization was induced by a unique 120° Y-type antiferromagnetic structure and was modulated by the magnetic field, nevertheless, it was difficult to achieve the electrically controlled magnetism. The sliding ferroelectricity was observed in bilayer VS 2 , [26] however, the environmental stability of atomically thin VS 2 was unsatisfactory. Ultrathin-layered CuCrS 2 and CuCrSe 2 were room-temperature multiferroics, and the ferromagnetism was stabilized by the enhanced carrier density and the vertical polarization-induced orbital shifting. [27,28] 2D multiferroics with magnetoelectric coupling combine the magnetic order and electric polarization in a single phase, providing a cornerstone for constructing high-density information storages and low-energy-consumption spintronic devices. The strong interactions between various order parameters are crucial for realizing such multifunctional applications, nevertheless, this criterion is rarely met in classical 2D materials at room-temperature. Here an ingenious space-confined chemical vapor deposition strategy is designed to synthesize atomically thin non-layered ε-Fe 2 O 3 single crystals and disclose the room-temperature long-range ferrimagnetic order. Interestingly, the strong ferroelectricity and its switching behavior are unambiguously discovered in atomically thin ε-Fe 2 O 3 , accompanied with an anomalous thicknessdependent coercive voltage. More significantly, the robust room-temperature magnetoelectric coupling is uncovered by controlling the magnetism with electric field and verifies the multiferroic feature of atomically thin ε-Fe 2 O 3 . This work not only represents a substantial leap in terms of the controllable synthesis of 2D multiferroics with robust magnetoelectric coupling, but also provides a crucial step toward the practical applications in low-energy-consumption electric-writing/magnetic-reading devices.