  Two-dimensional (2D) multiferroics attract intensive investigations because
of underlying science and their potential applications. Although many 2D
systems have been observed/predicted to be ferroelectric or ferromagnetic, 2D
materials with both ferroic properties are still scarce. By using
first-principles calculations, we predict that hole-doping can induce robust
ferromagnetism in 2D ferroelectric {\alpha}-In2Se3 due to its unique flat band
structure, and the Curie temperature (TC) can be much higher than room
temperature. Moreover, the doping concentration, strain, and number of layers
can effectively modulate the magnetic moment and the TC of the material.
Interestingly, strong magnetoelectric coupling is found at the surface of hole
doped multilayer {\alpha}-In2Se3, which allows non-volatile electric control of
magnetization. Our work provides a feasible approach for designing/searching 2D
multiferroics with great potential in future device applications, such as
memory devices and sensors.
