Supramolecular-based nanofibers, which successfully combine the unique properties of supramolecular interactions with the advantages of nanofibrous structure, are widely used in a variety of biomedical applications such as controlled drug delivery. Compared with traditional polymer nanofibers, supramolecular-based nanofibers can overcome the bottleneck of sensitivity because of the non-covalent binding modes, and therefore match the requirements of rapid and reversible response to the external stimuli. In addition, supramolecular-based nanofibers can achieve extra controllable and dynamic responsive (e.g. pH, temperature) functions in different environments. In this review, we retrospected and summarized the recent development of supramolecular-based nanofibers, focusing particularly on electrospun supramolecular nanofibers, while also touching on the advances of directly self-assembled supramolecular nanofibers without the use of electrospinning. Furthermore, we discussed the potential biomedical applications of supramolecular nanofibers. Finally, this review was concluded by elaborating upon individual reflection on the current situation, forecasting the future trend of this promising material.