Smart electrospun hybrid nanofibers represent a cutting‐edge class of functional nanostructured materials with unique collective properties. This review aims to provide a comprehensive overview of the applications of smart electrospun hybrid nanofibers in the fields of energy, catalysis, and biomedicine. Electrospinning is a powerful tool to fabricate different types of nanofibers’ morphologies with precise control over structure and compositions. Through the incorporation of various functional components, such as nanoparticles, nanomoieties, and biomolecules, into the (co)polymer matrix, nanofibers can be tailored into smart hybrid materials exhibiting responsiveness to external stimuli such as temperature, pH, or light among others. Herein recent advancements in fabrication strategies for electrospun smart hybrid nanofibers are discussed, focusing on different electrospinning tools aimed at tailoring and developing smart hybrid nanofibers. These strategies include surface functionalization, doping, and templating, which enable fine‐tuning of mechanical strength, conductivity, and biocompatibility. The review explores the challenges and recent progress in the development of smart hybrid nanofibers. Issues such as scalability, reproducibility, biocompatibility, and environmental sustainability are identified as key for improvement. Furthermore, the applications of smart nanofibers in biomedicine, environment, energy storage, and smart textiles underscore their potential to address the challenges in development of nanostructured materials for emerging technologies.