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Herein, this paper reports a facile method to prepare electrospun carbon nanofiber mats (ECNFMs) with high specific surface area and interconnected structure using polyacrylonitrile (PAN) as a precursor and novolac resin (NOC) as a polymer sacrificial pore‐making agent. Without additional treatment, the prepared ECNFMs have a highly porous structure because NOC decomposes in a wider temperature range than most polymer activators. The NOC content in the PAN nanofibers shows important effects on porosity. The BET specific surface area of ECNFMs reaches a maximum of 1468 m2 g−1 when the precursor nanofibers contained 30 wt% NOC (ECNFM‐3) after carbonization at 1000 °C. The supercapacitor device from ECNFM‐3 electrode and all‐solid‐state electrolyte shows excellent cycling durability and high specific capacitance: ≈99.72% capacitance retention after 10 000 charge/discharge cycles and ≈320 mF cm−2 at 0.25 mA cm−2. Furthermore, it shows a large energy density of ≈11.1 μWh cm−2 under the power density of 500 mW m−2. Activation of carbon nanofibers simply by the addition of NOC into precursor nanofibers can offer a handy way to prepare ECNFMs for high‐performance all‐solid‐state supercapacitors and other potential applications. [ABSTRACT FROM AUTHOR]