Background: There is little understanding on how brief relaxation practice and viewing greenery images would affect brain responses during cognitive tasks. In the present study, we examined the variation in brain activation of the prefrontal cortex during arithmetic tasks before and after viewing greenery images, brief relaxation practice, and control task using functional near-infrared spectroscopy (fNIRS). Method: This randomized controlled study examined the activation patterns of the prefrontal cortex (PFC) in three groups of research participants who were exposed to viewing greenery images (n = 10), brief relaxation practice (n = 10), and control task (n = 11). The activation pattern of the PFC was measured pre- and post-intervention using a portable fNIRS device and reported as mean total oxygenated hemoglobin (HbO μm). Primary outcome of the study is the difference in HbO μm between post- and pre-intervention readings during a cognitive task that required the research participants to perform arithmetic calculation. Results: In terms of intervention-related differences, there was significant difference in average HbO μm when performing arithmetic tasks before and after brief relaxation practice (p < 0.05). There were significant increases in average HbO μm in the right frontopolar cortex (p = 0.029), the left frontopolar cortex (p = 0.01), and the left orbitofrontal cortex (p = 0.033) during arithmetic tasks after brief relaxation practice. In contrast, there were no significant differences in average HbO μm when performing arithmetic tasks before and after viewing greenery images (p > 0.05) and the control task (p > 0.05). Conclusion: Our preliminary findings show that brief relaxation practice but not viewing greenery images led to significant frontal lobe activation during arithmetic tasks. The present study demonstrated, for the first time, that there was an increase in activation in neuroanatomical areas including the combined effort of allocation of attentional resources, exploration, and memory performance after the brief relaxation practice. Our findings suggest the possibility that the right frontopolar cortex, the left frontopolar cortex, and the left orbitofrontal cortex may be specifically associated with the benefits of brief relaxation on the brain.