• Pitch-derived soft carbons with tunable structures were synthesized by carbonization at 600–1400 °C, revealing clear correlations between carbon microstructure and potassium storage performance.
• The carbon obtained at 700 °C exhibited a high degree of disorder and large interlayer spacing, delivering a high reversible capacity of 329.4 mAh g−1 and an initial coulombic efficiency of 72.81%.
• The low-potential plateau capacity correlates with carbon crystal size, while the sloping region capacity is linked to the degree of structural disorder, providing mechanistic insights into K+ storage.
• The optimized carbon anode maintained a high capacity of 144.2 mAh g−1 at a high current rate of 5 C, demonstrating excellent rate capability for potassium-ion batteries.
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