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Black thermal control blankets have been widely used in spacecraft for eliminating stray light around high-resolution optical instruments. However, the limited absorption in visible light range, the fast degradation upon hyperthermal atomic oxygen (AO) in low Earth orbit (LEO), and the poor adhesion of black coatings with substrate confined their applications into board solar spectrum and multi-layer interface engineering. In this work, a nanocomposite polyimide film containing a trisilanolphenyl POSS, a dye of solvent black 34, and a carbon black of CABOT M800 has been designed. With an ingredient of 20 wt% POSS, 5 wt% dye, and 10 wt% carbon black, the nanocomposite polyimide film PPIBC10 exhibited an ultra-low transmittance near zero in the range 200–2000 nm, a low reflectance below 5% in UV range and below 2% in VIS-IR range, and a low erosion yield of 0.49 ± 0.11 × 10−24 cm3 atom−1 upon a 2.27 × 1020 atoms cm−2 hyperthermal AO exposure, with an absorptance of 0.983, an emissivity of 0.86, and a coefficient of thermal expansion of 20 ppm oC−1. SEM and XPS analysis indicated that a uniform SiO x passivating network was formed on surface upon the hyperthermal AO exposure. The tensile strength decreased with increasing additives, and kept stable upon the AO exposure, for there was only sub-micrometer in erosion depth. The thermal expansion coefficients of the nanocomposite films are comparable to that of Kapton, which benefits interface engineering. The small granularity of tens of micrometers and good solubility in poly(amic acid) of additives POSS, dye, and carbon black benefit potential manufacture. This study suggests an ultra-black AO durable polyimide film for potential applications in LEO. Image 1 • A nanocomposite polyimide film was designed with additives of a POSS, a dye, and a carbon black in poly(amic acid). • Bulk-phase black dye and carbon black reinforcements for ultra-low transmittance and reflectance in solar spectrum. • Bulk-phase POSS reinforcement for atomic oxygen resistance. • Comparable coefficient of thermal expansion to Kapton. • Small-granularity and soluble additives in polar solvent. [ABSTRACT FROM AUTHOR]