We aimed to compare psychophysiological responses in adults according to cognitive demand levels for horticultural activities to confirm the feasibility of horticultural activity for improving attention and emotional states. A total of 60 adults in their 20s were included in this crossover design study. Participants performed soil-mixing activities with 2 cognitive demand levels for 2 min each. Electroencephalography (EEG) and electrocardiography (ECG) were performed during these activities. After each activity, the semantic differential method (SDM) was used to evaluate the emotional states of the participants. EEG results revealed that relative fast alpha and low beta power spectrums in the frontal lobes were high during the activity with high cognitive demand compared to those during the low demand activity, which indicates activation in the prefrontal cortex. ECG results showed that during the high cognitive demand activity, the standard deviation of the RR intervals of male adults was high, indicating a high-stress resistance ability of the autonomic nervous system. However, as a result of the SDM, there were no significant differences in emotional states according to the level of activity difficulty. Therefore, this study confirmed the possibility that the intervention of horticultural activities of an appropriate difficulty did not negatively affect subjective emotional changes and could have a positive effect on the improvement of attention levels and emotional stability in adults.