Due to the current limitations of three-dimensional (3D) simulation graphics technology, mind wandering commonly occurs in virtual reality tasks, which has impeded it being applied more extensively. The right ventrolateral prefrontal cortex (rVLPFC) plays a vital role in executing continuous two-dimensional (2D) mental paradigms, and transcranial direct current stimulation (tDCS) over this cortical region has been shown to successfully modulate sustained 2D attention. Accordingly, we further explored the effects of electrical activation of the rVLPFC on 3D attentional tasks using anodal high-definition (HD)-tDCS. A 3D Go/No-go (GNG) task was developed to compare the after effects of real and sham brain stimulation. Specifically, GNG tasks were periodically interrupted to assess the subjective perception of attentional level, behavioral reactions were tracked and decomposed into an underlying decision cognition process, and electroencephalography data were recorded to calculate event-related potentials (ERPs) in rVLPFC. Thep-values statistically indicated that HD-tDCS improved the subjective mentality, led to more cautious decisions, and enhanced neuronal discharging in rVLPFC. Additionally, the neurophysiological P300 ERP component and stimulation being active or sham could effectively predict several objective outcomes. These findings indicate that the comprehensive approach including brain stimulation, 3D mental paradigm, and cross-examined performance could significantly lengthen and robustly compare sustained 3D attention.