Graphene‐like films (GLFs) are selectively deposited on the silicon oxide/silicon structures preirradiated with electrons at various electron energies and irradiation doses. These films demonstrate high conductivity and are used as a gate material for metal‐oxide‐semiconductor (MOS)‐based devices. It is shown that high‐quality capacitance–voltage characteristics of the GLF‐gated MOS structures can be obtained if both an energy and a dose are carefully tuned. Using the GLF‐gated MOS as a pseudo‐field effect transistor structure, a notable current modulation in the selectively grown GLF is observed.