“…Multiferroic materials, which possess two or more ferroic orders simultaneously, such as spontaneous electric polarization and magnetization in a single phase, have attracted more attention because of their intriguing physics and novel technological applications. − In particular, if these systems have magnetoelectric (ME) coupling effect, they could provide an useful avenue for the development of novel devices based on new functionalities such as control of the magnetic properties by means of electrical fields and vice versa. , Over the past decades, numerous single-phase multiferroics have been presented by advanced preparation techniques and first-principle calculations, such as ferroelectric-antiferromagnetic (Bi, Gd, Dy, Yb, Sm, La, and Lu) FeO 3 , − (Dy, Gd, and Tb) CrO 3 , , (Sr, Y, Dy, Tb, and Ho) MnO 3 , − and (Mn, Fe, Co) 2 Mo 3 O 8 , , ferroelectric–ferrimagnetic Fe 3 O 4 and MnCr 2 S 4 , , ferroelectric–ferromagnetic EuTiO 3 , and so on. − Unfortunately, the available materials are still lacking and elusive because of their antiferromagnetic nature or low working temperature ( T w ). Thus, it is vital to continue exploring new multiferroic materials possessing high T w , strong ferromagnetism, and a strong ME coupling effect for the practical application. , …”