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Dielectric film with ultrahigh thermal stability based on crosslinked polyarylene ether nitrile is prepared and characterized. The film is obtained by solution-casting of polyarylene ether nitrile terminated phthalonitrile (PEN-Ph) combined with post self-crosslinking at high temperature. The film shows a 5% decomposition temperature over 520 °C and a glass transition temperature ( T  g ) around 386 °C. Stable dielectric constant and low dielectric loss are observed for this film in the frequency range of 100–200 kHz and in the temperature range of 25–300 °C. The temperature coefficient of dielectric constant is less than 0.001 °C −1  even at 400 °C. By cycling heating and cooling up to ten times or heating at 300 °C for 12 h, the film shows good reversibility and robustness of the dielectric properties. This crosslinked PEN film will be a potential candidate as high performance film capacitor electronic devices materials used at high temperature.

Crosslinked polyarylene ether nitrile film as flexible dielectric materials with ultrahigh thermal stability