Shell‐isolated nanostructures, consisting of an inert shell and a plasmonic core, have recently been intensively explored for biosensing, catalysis, and nanoelectronics applications owing to their functional shells and unique plasmonic properties. Such designer shell‐isolated plasmonic nanostructures possess the potential to improve the detectability of biosensors and provide powerful platforms to explore in‐depth plasmon enhancement principles and finally boost significantly their photo(electro)catalytic efficiency. In addition, such structural optimization and interface nanoengineering promote solid developments of advanced nanoelectronics toward real applications, revealing new electron transport mechanisms and enabling exploration of new functional and integrated optoelectronic devices. In this overview, the state‐of‐the‐art progresses of shell‐isolated plasmonic nanostructures (SHIPNSs) in the field of biosensing, photo(electro)catalysis, and nanoelectronics is summarized, focusing on the superiority of the core–shell materials in exploration of biosensing, catalytic enhancement mechanisms, and electron transport principles. A brief overview of synthetic methods is introduced, and then the significant importance of shell‐isolated nanomaterials in fabrication and promising direction for future development and challenges are discussed.