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With the rapid development of nanotechnology, research interest in nanofibers has grown exponentially, especially for those prepared by electrospinning. Electrospun nanofibers are light weight with high surface-to-volume ratio, adjustable fiber diameter/morphology, and well-controlled functionality, making them a very important nanomaterial for various applications. Considerable effort has been devoted to improving electrospinning efficiency, controlling nanofiber structure, and finding their unique property and novel application. From the initial study that used a simple needle-based electrospinning setup, electrospinning has entered a new era of mass production from needleless apparatus and nonweb fibrous structure-like nanofiber yarns. This chapter provides an overview of electrospinning, its brief history, physical principle, advanced electrospinning setups, and functional applications. The advantages of electrospinning and nanofibers, their structures, and functionalities are discussed in detail.