Colloidal electrospinning is identified as a powerful tool for the fabrication of nonwoven nanofiber webs with increased functionality by the introduction of functional fillers into the webs. However, the use of this method is still limited due to minimal material diversity, low concentration of fillers, difficulty in mass production, and process difficulties. In this paper, syringeless electrospinning is suggested as an excellent method for colloidal electrospinning. Since the polymeric solution is supplied from the container through rotating drums, this method is relatively free from the precipitation of fillers present in the polymeric solution. Syringeless electrospinning provides a higher production rate than needle‐based electrospinning with simple process control. The syringeless technique makes it possible to expand the scope of the method to various polymers and inorganic fillers with sufficiently high filler concentrations. Herein, nonwoven nanofiber webs with a diverse combination of polymers (polyacrylonitrile (PAN), thermoplastic polyurethane (TPU), and polyvinylpyrrolidone (PVP)) and fillers (silica, titania, zirconia, activated carbons, and metal‐organic framework (MOF) crystals) are presented. Nonwoven nanofiber webs comprising PAN and UiO‐66‐NH2 MOF crystal are prepared for detoxification of a nerve agent simulant, diisopropyl fluorophosphate (DFP), as a representative example of applications.