Plasma polymerized styrene (ppS) thin films were prepared and used as gate insulator and tunneling layer in a floating-gate type organic memory device. To investigate feasibility of the ppS thin film for application in non-volatile organic memory, an organic thin film transistor (OTFT) and a floating-gate type organic memory device were fabricated. Current–voltage (I–V) characteristics of the OTFT and floating-gate type organic memory device were comparatively investigated, and hysteresis in the I–V characteristics of both devices was studied. A pseudo-charge-storage phenomenon was found for the ppS insulator thin film in the OTFT and floating-gate type organic memory device. The floating-gate type organic memory device revealed a reasonable hysteresis voltage of 27 V. It was confirmed that the ppS could be applied to fabricate an alternative floating-gate type organic memory device with promising memory function.