Composite thin films of BaTiO3 (BTO) and CoFe2O4 (CFO) on (001)-oriented SrTiO3 (STO) substrates were prepared by the spin coating technique using solutions of the corresponding metal cations in N,N-dimethylformamide/acetic acid. Ten and five individual coating steps for the bottom perovskite layer and the top ferrite layer resulted in thicknesses of 250 nm and 200 nm, respectively. X-ray diffraction (XRD) and Raman spectroscopy proved the formation of BaTiO3 and CoFe2O4 without any detectable impurities. Rocking curve scans, reciprocal space mapping (RSM) and pole figures clearly demonstrated the epitaxial growth of both the perovskite and the ferrite layer, i.e. STO(001)[100]parallel to BTO(001)(100]parallel to CFO(001)[100]. Furthermore, scanning electron microscopy (SEM) investigations revealed smooth interfaces and dense films. From atomic force microscopy (AFM) surface scans, a roughness of about 8 nm was deduced. A saturation magnetization of about 350 emu.cm(-3) was found and the samples showed only a small magnetic anisotropy.