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A series of novel polyimides (PIs) based on N,N-di(4-aminophenyl)-2-amino-9,9-dimethylfluorene and various dianhydrides were synthesized. These PIs were amorphous and readily soluble in many solvents. They displayed outstanding thermal stability and high glass transition temperatures (269–374°C). The polymer films showed reversible electrochemical redox and satisfactory electrochromic performance with long-term stability, high coloration efficiency, and acceptable switching times. The PI derived from 1,2,4,5-cyclohexanetetracarboxylic dianhydride exhibited maximum fluorescence at 400 nm with quantum yields up to 28.1%. Furthermore, the fluorescence can be effectively electroswitched between “on” and “off” states, exhibiting a high contrast ratio of 75.