Summary: Polyimide‐mica hybrid films were prepared via ultrasonic dispersion and in situ polymerization process from a solution of a polyimide precursor and mica in N,N‐dimethylacetamide, and their structure was characterized by FTIR and XRD techniques. The dependence of dielectric properties, such as dielectric constant and electrical breakdown strength, of the hybrid films on the content of mica was studied at room and cryogenic temperatures. The results show that the dielectric constant of PI‐mica hybrid films decreases with the increase of the mica content at temperatures from −150 to 150 °C and at frequency range from 1 kHz to 1 MHz. It was found that the cryogenic electrical breakdown strength of the PI‐mica hybrid films could meet the requirements of cryogenic insulating materials.Effect of frequency on the dielectric constant of PI‐mica hybrid films at 140 °C at the frequency from 1 kHz to 1 MHz.magnified imageEffect of frequency on the dielectric constant of PI‐mica hybrid films at 140 °C at the frequency from 1 kHz to 1 MHz.