Experience of natural landscapes in virtual reality (VR) is increasingly seen as an effective alternative to being in real green spaces, for both neurorehabilitation and general emotional well-being. In our paper, we explore how the individual differences in the “pre-tuning” processes of brain activity are affected by the Emotional Intelligence traits. We subjected 20 student participants to 4 experimental conditions, which included the virtual forest walk in 2D (computer screen) and 3D (VR headset). We registered and analyzed the subjects’ electroencephalograms (EEGs) with the focus on Delta, Theta, Alpha2 and Beta2 bands that are considered the most informative ones with respect to perception of nature. The results suggest that the contribution of positive expressiveness (EI1) to the “pre-tuning” of the activity of the cerebral cortex both in the low-frequency Delta band and the high-frequency Beta2 was the most pronounced. Interestingly, the spatial allocation of the correlations for the negative expressiveness component (EI2) was rather similar to the ones for EI1. A decrease in the amplitude of Alpha biopotentials in the parietal cortex of the right hemisphere during the “pre-tuning” corresponded to higher values for emotion-based decision-making (EI4). EI4 was associated also with the Delta decrease in anterior cortex for the 2D format, whereas for the 3D we discovered positive relationships between EI1 and Beta2 rhythm. The results of our study contribute to the understanding of spatial and frequency patterns in brain neural networks associated with the experience of virtual nature in various conditions.