Researchers have developed many types of nanoscale materials with different properties. Among them, nanofibers have recently attracted increasing interest and attention due to their functional versatility and potential applications in diverse industries, including tapes, filtration, energy generation, and biomedical technologies. Nanolayer coextrusion, a novel polymer melt fiber processing technology, has gradually received attention due to its environmental friendliness, efficiency, simplicity and ability to be mass-produced. Compared with conventional techniques, nanolayer coextruded non-woven nanofibrous mats offer advantages such as a tunable fiber diameter, high porosity, high surface area to volume ratio, and the potential to manufacture composite nanofibers with different components to achieve desired structures and properties. Dozens of thermoplastic polymers have been coextruded for various applications, and the variety of polymers has gradually continued to increase. This review presents an overview of the nanolayer coextrusion technique and its promising advantages and potential applications. We discuss nanolayer coextrusion theory and the parameters (polymer and processing) that significantly affect the fiber morphology and properties. We focus on varied applications of nanolayer coextruded fibers in different fields and conclude by describing the future potential of this novel technology.