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In the current work, a series of black polyimide (PI) films with excellent thermal and dimensional stability at elevated temperatures were successfully developed. For this purpose, two aromatic diamines including 4,4'-iminodianline (NDA) and 2-(4-aminophenyl)-5- aminobenzimidazole (APBI) were copolymerized with pyromellitic dianhydride (PMDA) to afford PIs containing imino groups (-NH-) in the molecular structures. The referenced PI film, PI-ref, was simultaneously prepared from PMDA and 4,4'-oxydianiline (ODA). The introduction of imino