Gallium arsenide nanowires (GaAs NWs) formed by anodic etching show an electrically semi-insulating behavior because of charge carrier depletion caused by high interface state density. Here, we demonstrate the gate modulation of an anodically etched GaAs NW random network. By applying a reverse bias voltage after anodic etching of bulk GaAs, hydrogen ion exposure of the depleted NW region occurs, and then the interface state density is possibly decreased owing to the reduction in the amount of excess As generated at the interface between the amorphous Ga2O3 and GaAs layers. Consequently, the drain current of the thin-film transistor (TFT) with the GaAs NW random network was increased and was changed by the gate voltage. In contrast, the random network film remained in the insulator in the absence of reverse electrolysis treatment. The TFT performance is still insufficient but may be improved by optimizing the hydrogen ion exposure conditions.