Self-care is a critical component and considered a core foundational competency for doctoral students in the field of psychology. It is an ethical imperative to maintain adequate self-care to prevent burnout and negative outcomes to those receiving health-care services. Self-care is also related to the professional values of psychology, specifically, beneficence and nonmaleficence. However, little research has explored the topic. One reason that may contribute to the scant research is the lack of a valid tool to measure self-care behaviors. In the first study, we developed and validated a self-care instrument with 232 doctoral students in programs accredited by the American Psychological Association across different stages of the developmental trajectory. A pilot study (n = 28) provided feedback on item content and suggestions for improvement. In the second study, the refined self-care instrument, the Self-Care Behavior Inventory, was used, along with the Maslach Burnout Inventory–Human Services Survey (Schaufeli, Leiter, & Maslach, 2009), the Perception of Competence Scale (Williams & Deci, 1996), the Flourishing measure (Diener et al., 2010), and the Contributors to Distress measure (Carter & Barnett, 2014). Exploratory factor analyses revealed a 3-factor model with Cognitive–Emotional–Relational, Physical, and Spiritual components underlying the construct of self-care. Limitations of the present study and implications for training programs and trainees are discussed, as are suggestions for future research.