Equine-assisted services (EAS) are used for civilian and military trauma survivors to reduce depression and posttraumatic stress symptoms. While early scientific evidence supports the benefits of EAS, the neurophysiological mechanisms underlying these benefits are unknown. The specific aims of this exploratory study were to determine (1) whether functional near-infrared spectroscopy (fNIRS) neuroimaging can be used to explore neural responses of EAS veteran participants and (2) the correlation between neural responses and psychological outcomes of the participants interacting with equines. Fifteen veterans participated in a 2-day EAS program consisting of four randomized activities. An fNIRS sensor cap was used to measure the oxygenated (O2Hb), deoxygenated (hHb), and total hemoglobin (tHb) of the participants during each activity. The results indicated no significant differences for O2Hb and tHb across the visits or activities, however, a significant difference in hHb was observed. There was an increase in hHb during the activities that included an equine, which indicated a greater cognitive load and attention. Further, data from pre-/post-psychometric assessments showed a significant improvement in participants’ trait anxiety, psychological flexibility, and positive and negative affect after interacting with the horse. Preliminary data revealed a potential association between the cognitive attention and psychological health of participants during an EAS session.