An abundance of literature on caregivers of individuals with dementia has been written since the mid-1980s. However, most of this literature focused on the experience of stress, burden, and depression in caregivers, thus excluding the grief experience that also accompanies the caregiving experience. The purpose of this multimethod study is to describe the lived experience of 44 spouses and adult children who are caregivers of persons with Alzheimer's disease and related dementias (ADRD) and scored high on the Marwit and Meuser Caregiver Grief Inventory, Short Form (MM-CGI-SF). This study presents qualitative results from a mixed-methods descriptive study (N = 201). Seven themes emerged from the qualitative data that detailed the caregiving experience of the individuals with high grief: (a) yearning for the past, (b) regret and guilt, (c) isolation, (d) restricted freedom, (e) life stressors, (f) systemic issues, and (g) coping strategies. The first 2 themes reflect grief reactions, whereas isolation, restricted freedom, life stressors, and systemic issues possessed elements of both grief and caregiver burden and stress. Coping strategies used by this group of caregivers included spiritual faith, social supports, and pets. Quantitative analysis confirmed that these themes are unique to individuals with high levels of grief compared with those with moderate/low levels of grief, except for the coping strategies of social support and spiritual faith. Caregivers with high levels of grief may benefit from supportive interventions that are based on reducing feelings of isolation, lack of freedom, and increased guilt and regret, while also addressing feelings of loss. Interventions that facilitate building a supportive network are suggested. Using a screening tool such as the MM-CGI-SF will help in identifying caregivers with high levels of grief who may be in need of additional support.