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This Letter reports on the deposition of a conductivity-switching polyimide film as a recording medium formed by molecular layer deposition (MLD). It also reports on the electrical modification on it using a scanning probe microscope (SPM). The polyimide film is uniformly deposited on an Au surface by MLD. As the result of the electrical modification, highly conductive dots pattern with a narrow pitch of approximately 50 nm is successfully defined by applying pulsed voltages. The current ratio of the electrical modified area to unmodified area reached 300 at least.