This study aimed to compare the brain activity and emotional states of elementary school students during horticultural and nonhorticultural activities. A total of 30 participants with a mean age of 11.4 ± 1.3 years were included. This experiment was conducted at Konkuk University campus in Korea. Participants performed horticultural activities such as harvesting, planting, sowing seeds, and mixing soil. Nonhorticultural activities included playing with a ball, solving math problems, watching animation videos, folding paper, and reading a book. The study had a crossover experimental design. Brain activity of the prefrontal lobes was measured by electroencephalography during each activity for 3 minutes. On completion of each activity, participants answered a subjective emotion questionnaire using the semantic differential method (SDM). Results showed that relative theta (RT) power spectrum was significantly lower in both prefrontal lobes of participants when engaged in harvesting and reading a book. The relative mid beta (RMB) power spectrum was significantly higher in both prefrontal lobes when participants engaged in harvesting and playing with a ball. The ratio of the RMB power spectrum to the RT power spectrum reflects concentration. This ratio increased during harvesting activity, indicating that children’s concentration also increased. The sensorimotor rhythm (SMR) from mid beta to theta (RSMT), another indicator of concentration, was significantly higher in the right prefrontal lobe during harvesting than during other activities. Furthermore, SDM results showed that the participants felt more natural and relaxed when performing horticultural activities than nonhorticultural activities. Horticultural activities may improve brain activity and psychological relaxation in children. Harvesting activity was most effective for improving children’s concentration compared with nonhorticultural activities.