Potassium-ion batteries (PIBs) are of academic and economic significance, but still limited by the lack of highly active electrode materials for de-/intercalation of large-radius K ions. Herein, an interconnected nitrogen/sulfur co-doped carbon nanosheep bundle (N/S-CSB) was proposed as the potassium ions storage material. The rich co-doping of nitrogen/sulfur of N/S-CNB with three-dimensional hierarchical bundled array structure yields distensible interlayer spaces to buffer the volume expansion during K⁺ insertion/extraction, offers more electrochemical active sites to obtain a high specific capacity, and provides efficient channels for fast ion/electron transports. Therefore, the N/S-CSB anode achieved high reversible specific capacity of 365 mAh/g obtained at 50 mA/g after 200 cycles with a coulombic efficiency (CE) close to 100%, high rate performance and long cycle stability. Moreover, the in-situ Raman spectra indicated outstanding reaction kinetics of as-prepared N/S-CSB anode.