The majority of research on religion and mental health has been conducted on Western Christians. Religion and mental health are often measured in different ways across studies, making it difficult to understand the complex role of faith on mental health outcomes. Using a global Muslim sample, this study investigates the association between a holistic measure of religiosity and various measures of mental health and mental illness. Multiple regression was used to analyze the demographic (e.g., age, gender, marital status, education) and psychospiritual correlates (holistic religiosity, religious doubts, and uncertainty intolerance) of five mental health outcomes, including depression, anxiety, purpose in life, life satisfaction, and subjective well-being. A large sample of English-speaking Muslims globally was attained. We found that holistic religiosity was a significant predictor of all mental health outcomes (N = 3,551). Uncertainty intolerance was the strongest predictor of psychological distress (i.e., anxiety and depression), whereas religiosity was the strongest predictor of thriving outcomes (i.e., life satisfaction, well-being, and purpose in life). Religious doubt was also a significant predictor of multiple mental health outcomes. Religiosity is a multifaceted construct that includes various beliefs and behaviors. Mental health is also an ambiguous term that may refer to both aspects of thriving and illness. The proper conceptualization and measurement of religiosity and mental health are essential to understanding the complex relationship between religion and mental health.