Previous studies designing Virtual Reality (VR) suggest that interaction with virtual pets can increase users’ sense of presence, which consequently could lead to technological interventions for well-being and mental health. However, further studies are needed to assess and understand the effects of VR on users’ emotional states. In this study, informal caregivers of People with Dementia or related conditions used VR to navigate in a virtual forest (a Virtual Natural Environment - VNE) and interact with a virtual dog (petting vs. throwing a bone). Through a mixed-methods approach, we found increased energy and decreased tension when participants interacted with the virtual dog. Feelings of joy, companionship, and security were reported by participants after the interaction with the virtual dog in VR. Participants expressed interest in incorporating virtual dog interaction in VR into their daily routines to help them to cope with stressful situations.