This chapter intends to review the state of the art of a new nanomaterial generation based on electrospun composite nanofibers for dye removal from wastewater. Natural polymer-based nanofibers, nanofibers with unique morphology, and carbon nanofibers were comprehensively reviewed as capable carriers for a broad spectrum of functional materials such as metal oxides, zeolite, graphene and graphene oxide (GO), and metal-organic frameworks (MOFs) in the application of dye removal. The various nanostructures, adsorption capacity, advantages, and drawbacks were discussed along with mechanistic actions in the adsorption process and photocatalytic performance that emphasize current research development, opportunities, and challenges. The chapter covers multiple intriguing topics with in-depth discussion and is a valuable reference for researchers who are working on nanomaterials and the treatment of colored waters.