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Polyimides have a long history of use in space missions, with Kapton® being the first polymer material to touch the surface of the Moon. Polyimides offer remarkable mechanical strength, superior thermal stability, and resistance to radiation, chemicals, and wear, and as such are often serve as a thermal barrier and a protective layer against extreme radiation and temperatures in multi-layer insulation systems. While the use of Kapton® in spacesuits dates back to the two aluminised Kapton® layers used in the spacesuits in the Apollo 11 mission, the potential uses of polyimides in the design of spacesuits remain underexplored, particularly considering the advancement made in the development of high-performance polyimide-based composites. This review explores the opportunities that emerge when the desirable properties of polyimides are combined with that of nanomaterials, specifically carbon nanomaterials, to produce strategic material combinations that promise to achieve enhanced thermal and mechanical properties, improved resistance to abrasion and puncture, and potentially reduced weight compared to traditional spacesuit materials. In turn, these advancements will contribute to the development of next-generation spacesuits that offer superior comfort, protection, and astronaut mobility during extravehicular activities.