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Metallic nanostructures and thin films are fundamental building blocks for next‐generation nanophotonics. Yet, the fixed permittivity of pure metals often imposes limitations on the materials employed and/or on device performance. Alternatively, metallic mixtures, or alloys, represent a promising pathway to tailor the optical and electrical properties of devices, enabling further control of the electromagnetic spectrum. In this Review, a survey of recent advances in photonics and plasmonics achieved using metal alloys is presented. An overview of the primary fabrication methods to obtain subwavelength alloyed nanostructures is provided, followed by an in‐depth analysis of experimental and theoretical studies of their optical properties, including their correlation with band structure. The broad landscape of optical devices that can benefit from metallic materials with engineered permittivity is also discussed, spanning from superabsorbers and hydrogen sensors to photovoltaics and hot electron devices. This Review concludes with an outlook of potential research directions that would benefit from the on demand optical properties of metallic mixtures, leading to new optoelectronic materials and device opportunities. [ABSTRACT FROM AUTHOR]