BACKGROUND: There is growing attention given to the spiritual needs of dying patients and long-term care (LTC) facilities are common settings in which patients receive care as they approach death. OBJECTIVES: To describe the sources of support, the structure and processes of spiritual care in LTC, and examine the relationship between these components and family ratings of overall care. RESEARCH DESIGN: After-death interviews of family members of decedents. SUBJECTS: Family members of 284 decedent residents from a stratified sample of 100 residential care/assisted living facilities and nursing homes in Florida, Maryland, New Jersey, and North Carolina. MEASURES: Interview items included sources of spiritual support, processes of spiritual care, and the impression of overall care (4 = very good, 3 = good, 2 = fair, 1 = poor) for decedents. Facility-level data included demographics, counseling by clergy, on-site religious services, hospice services, and hospice unit. RESULTS: Most decedents (87%) received assistance with their spiritual needs and those who received spiritual care were perceived by family members to have had better overall care (3.59 vs. 3.25, P = 0.002). Family ratings of care ratings were higher for those who received spiritual support or care from facility staff when compared with those who did not (3.76 vs. 3.49, P < 0.001) and better care was associated with the facilitation of individual devotional activities (3.87 vs. 3.53, P = 0.001). CONCLUSIONS: Spiritual support and care are associated with better overall care at the end of life for LTC residents, and interventions to improve this type of care may best target interactions between residents and facility staff.