Comparing the performance of recently reported electrospun carbon nanofiber (CNF)-based supercapacitors, which use binders, we are reporting a binder-free high-performance supercapacitor based on porous bubbled surface carbon nanofibers (BCNFs). BCNFs have been synthesized by using a KIT-6 silica template-assisted electrospinning process, and they exhibit a high discharge specific capacitance of 287 F g−1 (79.7 mAh g−1). Brunauer−Emmett−Teller and FESEM analyses reveal that BCNFs have a large accessible surface area (593 m2 g−1) and well-developed pore structures, leading to a high specific capacitance value. Furthermore, a BCNF supercapacitor exhibits good cyclic stability with improved capacity retention in aqueous electrolyte. The use of electrospinning and a hard template method for the synthesis avoids the use of aggressive materials and complicated activations, thereby making it an industry-compatible process for large-scale production. The present study, demonstrating the successful synthesis of BCNFs, is a major step ahead in the direction of developing new materials for binder-free supercapacitors, which hold enormous potential for high-performance energy storage devices. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim