Single and multilayer films of La0.67Sr0.33MnO3 and CoFe2O4 were deposited by spin-coating. The all-alkoxide precursors allowed inorganic gel films of extreme homogeneity to be formed and converted to phase pure complex oxides at low temperatures. La0.67Sr0.33MnO3 films were made with La- and Ca-methoxy-ethoxides and Mn19O12(moe)(14)(moeH)(10) as precursors at 800 degrees C. The CoFe2O4 films were obtained at extremely low 275 degrees C, using a new CoFe2-methoxyethoxide precursor. The decomposition and microstructural development on heating was described by TG, TEM, XRD and IR spectroscopy. XRD showed no spurious phases and the unit-cell dimensions coincided quite well with literature values of the targeted phases. The structural, magnetic and electronic properties of these films established their phase purity and high quality with physical properties comparable to films deposited by physical deposition methods. The magnetic and magneto transport results are presented for single, bi- and tri- layer structures. The magnetically soft La0.67Sr0.33MnO3 layer was exchange coupled to the magnetically hard CoFe2O4 layer, giving rise to interesting switching behaviour in magnetism and magneto-transport properties.