A (001)-epitaxial-BiFeO3/CoFe2O4 bilayer was grown by self-assembly on SrTiO3 (100) substrates by just coating a mixture precursor solution. The thickness ratio of the bilayer could be controlled by adjusting the composition ratio. For example, a BiFeOx:CoFe2Ox = 4:1 (namely Bi4CoFe6Ox) mixture solution could make a total thickness of 110 nm divided into 85-nm-thick BiFeO3 and 25-nm-thick CoFe2O4. Self-assembly of the bilayer occurred because the perovskite BiFeO3 better matched the lattice constant (misfit approximately 1%) and crystal symmetry of the perovskite SrTiO3 than the spinel CoFe2O4 (misfit approximately 7%). The magnetic domains of the hard magnet CoFe2O4 were switched by the polarization change of BiFeO3 due to an applied vertical voltage, and the switched magnetic domain size was approximately 100 nm in diameter. These results suggest that self-assembled BiFeO3/CoFe2O4 bilayers are interesting in voltage driven nonvolatile memory with a low manufacturing cost.