Over the past decades, research has emerged in the health care field to demonstrate that patient satisfaction is an important asset for hospital quality improvement. Patient’s satisfaction and experiences are increasingly used as indicators of quality in health care. This study aimed at assessing service use satisfaction with psychiatric and mental health care services at Federal Neuropsychiatric Hospital Calabar, Cross River State, Nigeria. The specific objectives were to determine service users’ satisfaction with psychological care, physical care, social care and satisfaction with the therapeutic and physical environment care. The study was a descriptive cross sectional survey and instrument for the data collection was adapted Newcastle satisfaction with Nursing scales (NSNS) questionnaire. Two hundred and seventy one respondents were used for the study. Data was analyzed using a statistical software package for Social Science (SPSS) version 20.0, the mean, standard deviation and one way ANOVA was used to established relationship between demographic variables and services users’ satisfaction with psychological, physical and social care. Findings revealed that the means and standard deviation of psychological care was (X = 3.83, SD = 0.77). Mean and standard deviation on service users’ satisfaction with physical care was (X = 3.52, SD = 0.93); social care was (X = 3.96, SD = 0.74); while the mean and standard deviation on service users’ satisfaction with therapeutic and physical environment was (X = 4.00, SD = 0.82). It was recommended that seminar and training of nurses on spiritual care should be organized by the continuing educational unit of the hospital to update their knowledge on areas not satisfied by patients.