Abstract Polyimide hollow microspheres (PIHMs) possess lightweight and excellent thermal resistance, making them highly valuable for various applications in aerospace, catalysis, and irradiation. Co‐polymerized PIHMs (PIHMBMDs) are fabricated through powder foaming combined with a gradient heating strategy in this work. The diameter of PIHMBMDs ranged from 364 to 1230 µm, which can be designed by regulating the size of polyester ammonium salts (PEASs). The PIHMBMDs possess intact morphology with a breakage rate of 3%–10% and low bulk density with a density ranging from 28.3 to 62.9 kg m−3. Furthermore, PIHMBMDs exhibit excellent thermal properties with a 5% weight loss temperature and glass transition temperature of 525.0 and 282.5 °C, respectively, making it an ideal material for fabricating lightweight and high‐temperature‐resistant multifunctional composites. Moreover, the proposed method is simple, efficient, and easily scalable, which is suitable for industrial applications to manufacture large quantities of PIHMs.
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