Flexible capacitors are a promising power source for foldable and biological electronic devices. Although various materials and device structures have been explored, they are still limited by low energy densities and slow rate capabilities compared to their rigid counterparts. Here, asymmetric carbon nanohorns are proposed as an active material to fabricate flexible solid‐state carbon wire (CW)‐based electrochemical supercapacitors (ss‐CWECs) which exhibit high power density and ultra‐low cutoff frequency. By controlling the electric arc reaction at low temperature (77 K), asymmetric single‐wall carbon nanohorns (SWCNHs) are synthesized with high yield. Based on microscopy and electrochemical characterization, the fundamental reaction mechanism in polyvinyl‐based electrolyte system is elucidated, as being associated with deprotonation reaction at acid, base, and elevated temperature conditions. Additionally, by using activated carbon, multi‐walled carbon nanotubes, and SWCNHs as hybrid electrode materials (5:1:1), remarkable specific length capacitance of 48.76 mF cm−1 and charge–discharge stability (over 2000 times cycles) of ss‐CWECs are demonstrated, which are the highest reported to date. Furthermore, a high‐pass filter for eliminating ultra‐low electronic noise is demonstrated, which enables an optical Morse Code communication system to be operated. Current results confirm the SWCNHs as promising materials for high‐performance soft electronics and energy storage applications.