3091wileyonlinelibrary.com magnetic, ferroelectric, piezoelectric, and multiferroic behaviors. [1][2][3][4][5] Nanocomposite oxides, with heterogeneous structures, can enable combinations of useful properties in one fi lm, and such fi lms can be formed by codeposition of two dissimilar phases. A notable example is the vertical nanocomposites formed from a spinel and a perovskite phase, such as BiFeO 3 -CoFe 2 O 4 grown on (001) SrTiO 3 which consist of columnar crystals of the spinel within a perovskite matrix, both epitaxial with the substrate. These have shown magnetism, ferroelectricity, and magnetoelectric coupling, [5][6][7][8] and, moreover, the locations of the spinel pillars on the substrate can be guided using a template. [12][13][14] The selfassembled fi lms are conveniently grown using pulsed laser deposition (PLD) from a single target or by alternating deposition from two different targets. Nanocomposite fi lms have also been produced consisting of metallic nanostructures in an oxide matrix, including Co x Ni 1-x alloy nanowires, Co nanocrystals, nanofi bers, or Fe nanorods embedded in a CeO 2 , TiO 2 , perovskite or other oxide matrix. [15][16][17][18][19] For example, metallic Cu nanopillars or nanoparticles in an oxide matrix have been reported for plasmon resonance studies and for battery electrodes. [20][21][22] The vertical nanocomposite fi lms reported to date comprise two different phases, but additional functionalities and crosscoupling of properties may be possible in nanocomposites with more than two phases. Three-phase oxide nanocomposites consisting of La 2 O 3 , SrO, and Co 2 O 3 were reported previously [ 23,24 ] but there has been no report on three-phase nanocomposites showing a vertically oriented epitaxial growth analogous to that seen in two-phase nanocomposites. Other examples of selfassembled oxide nanostructures include SrO x and (La,Sr)O x nanodots at the interface of Sr(Ti,Fe)O 3 and La 0.7 Sr 0.3 MnO 3 thin fi lms, which formed as a consequence of strain relaxation and electrostatic and elastic interactions, [ 25,26 ] and compositional heterogeneities which were found to develop in perovskite fi lms due to cation size and charge effects. [ 27 ] In this article, we describe the growth of a three-phase self-assembled epitaxial nanocomposite thin fi lm, denoted nc-STCu (nanocomposite-STCu), consisting of metallic Cu nanorods surrounded by a rocksalt-structured SrO oxide shell within a matrix of a Sr(Ti,Cu)O 3-δ perovskite phase. We then discuss the formation of a nanoporous oxide fi lm by