Architecture‐Driven Functional Coupling in Vertically Aligned Nanocomposites

ABSTRACT Vertically aligned nanocomposites (VANs) are self‐assembled thin‐film architectures in which phase distribution, interfacial density, and strain fields are defined concurrently during growth. Nanoscale vertical alignment and coherent interfaces generate anisotropic confinement and directional connectivity, thereby modifying ionic, electronic, optical, and magnetic responses across oxide, oxide‐metal, oxide‐nitride, and oxide‐alloy systems. This review examines how growth kinetics, elastic mismatch, and interfacial energetics control pillar morphology, defect distribution, and transport anisotropy in VAN platforms. Studies spanning electrochemical electrodes, dielectric materials, and magneto‐optical systems demonstrate enhanced oxygen exchange kinetics, anisotropic permittivity, strain‐stabilized phases, and coupled magnetic–optical behavior arising from architectural control. By correlating structural parameters with functional outputs, the literature establishes VANs as a versatile strategy for engineering coupled phenomena in complex oxides. Emerging design guidelines and open challenges are discussed to outline future directions for energy conversion and nanoelectronic applications.