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Multilayer (14 layers, 115–122 nm thick each) BiFeO3/CoFe2O4/substrate (BFO/CFO) and CoFe2O4/BiFeO3/substrate (CFO/BFO) nanocomposites were obtained by the method of sol-gel synthesis. It is shown that all samples of the obtained nanocomposites have multiferroic properties at room temperature. At the same time, there is a clearly demonstrated effect of the layering order on the values of remnant polarization and magnetization of these samples. This influence originates from the much smaller size of the crystallites in the BiFeO3 layers for the samples deposited in order (BFO/CFO) at various annealing temperatures (700, 725, and 750 °C). [ABSTRACT FROM AUTHOR]