Creating more pleated and collapsed structures for carbon‐based electrode materials is an important measure to enhance the performance of supercapacitors. Herein, a polymer formed by the aldimine reaction of terephthalaldehyde and aminopropyltriethoxysilane was utilized as the carbon source, and tetraethoxysilane was added as a silica additive to achieve the wrinkled structure on hollow carbon spheres. The silica had a significant modulating effect on the structure of the obtained wrinkled hollow carbon sphere (WHCS), which displayed a visible pleated structure, hollow structure, high specific surface area, and pore volume. As an electrode material for supercapacitors, WHCS exhibits excellent performance with a capacitance of 312 F ⋅ g−1 and remarkable cycle life stability, demonstrating its great potential for use in supercapacitors.
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