Food aroma molecules have the potential to influence people's emotions through the olfactory pathway and are anticipated to emerge as a new method for regulating emotional states, owing to their simplicity and high acceptance. Current research on food aroma predominantly centres on the physicochemical properties and formation mechanisms of aroma components, neglecting the effects of aroma molecules in emotional regulation. Moreover, the evaluation of pleasantness, a pivotal dimension of emotions, lacks objective assessment methods. In this study, sensory assessments of pleasantness for 12 aroma compounds were gathered from 45 subjects, and their correlation with the brain's activity responses in the left frontal‐temporal lobe (LFT) and right frontal‐temporal lobe (RFT) using electroencephalogram (EEG) signals was analysed. The results revealed a close relationship between brain activity in the LFT and the perception of aroma pleasantness. Furthermore, a substantial correlation was observed between the α, β and γ frequency bands in the LFT and the subjective pleasantness scores. These findings demonstrate that the LFT plays a critical role in evaluating the pleasantness of aroma molecules, and that changes in the power of the α, β and γ bands serve as important evaluation indicators. Consequently, this method offers a new objective means for assessing pleasantness to find higher pleasantness aroma molecules and the emotional regulation of food aroma.