polarization is very small (0.1 µ C cm −2 at ≈90 K) or it is even paraelectric. [ 4 ] In BFO, strong FE behavior (Ferroelectric transition temperature, T C,FE ≈ 1103 K) coexists together with antiferromagnetism (AFM). BFO has an incommensurate cycloidally modulated G-type AFM structure with a large period of 62 nm (Néel temperature, T N ≈ 650 K). [ 5,6 ] Despite having ferroelectric and magnetic ordering at high temperatures, BFO has drawbacks for practical applications. Most notably the weak FM-like magnetic behavior results from destruction of its incommensurate magnetic structure leading to AFM. [ 6 ] With strong ferromagnetic behavior in BMO and strong ferroelectric behavior in BFO, various studies have suggested combining BMO and BFO in order to achieve room-temperature (RT) multiferroicity. [7][8][9][10] One approach is to modify the local spin confi guration of Fe by chemical doping at the B -site. [ 8,9 ] By 50% doping, this simple concept could result in ordered double perovskite ferrites of Bi 3+ 2 Fe6 (TM = transition metal: Cr, Mn, Co, Ni, and Cu) giving antiferromagnetically coupled high spin state of the TM and Fe. However, this concept has not been widely realized due to the lack of cation ordering as a result of negligible differences in ionic valences and ionic radii. [11][12][13][14][15] On the other hand, disordered double perovskites (notably BiFe 0.5 Mn 0.5 O 3 (BFMO) and Bi 2 CoMnO 6 (BCMO)) show a strongly enhanced T C albeit with lower magnetic moment than expected for the ordered structure. [ 16,17 ] Pálová et al. extended the idea of ordered double perovskites by theoretically studying BFMO with an ordered nanoscale checkerboard structure (NCB-BFO/BMO, see Figure 1 a), i.e., columnar B -site ordering. [ 10 ] Their calculations predict that an ordered NCB-BFO/BMO would be ferroelectric and ferrimagnetic (FiM) with M S of 3.8 µ B /Fe-Mn pair and T C of 406 K, as a result of magnetic ordering arising from the superexchange coupling between the neighboring AFM-Fe and FM-Mn. [ 10 ] Unfortunately, spontaneous columnar B -site ordering is not expected and high quality growth of artifi cial 1:1 BFO/BMO superlattices along the 〈110〉 direction is very hard.