Abstract Nanocomposite thin films, comprising two or more distinct materials at nanoscale, have attracted significant research interest considering their potential of integrating multiple functionalities for advanced applications in electronics, energy storage, photonics, photovoltaics, and sensing. Among various fabrication technologies, a one-step pulsed laser deposition (PLD) process enables the self-assembly of materials into vertically aligned nanocomposites (VANs). The demonstrated VAN systems include oxide-oxide, oxide-metal, and nitride-metal VAN films and their growth mechanisms are vastly different. These complexities pose challenges in the designs, materials selection, and prediction of the resulted VAN morphologies and properties. The review examines the key roles that surface energy plays in the VAN growth and provides a generalized materials design guideline combining the two key factors of surface energy and lattice strain / mismatch, along with other factors related to growth kinetics that collectively influence the morphology of VAN films. This review aims to offer valuable guidelines for future material selection and microstructure design in the development of self-assembled VAN films.
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