Background: There is universal agreement on the essential role of critical thinking in nursing practice. Most studies into this topic have provided descriptive statistical information and insights on related external factors such as educational environment and teaching strategies. However, there has been limited research into the psychological factors that may predict the disposition of students toward critical thinking. Purpose: This study explored the relationship between the disposition of nursing students toward critical thinking and their mental self-supporting ability to obtain a profile and determine the psychological predictors of critical thinking. Methods: A cross-sectional descriptive study was conducted in 2013 using a convenience sample fromfour nursing schools. Four hundred six Chinese nursing undergraduates completed two questionnaires including (a) the California Critical Thinking Disposition Inventory (Chinese version) and (b) the Mental Self-Supporting Questionnaire for University Students. Pearson’s correlation and linear regression analysis were used to investigate the relationship between these two variables and the predicted positive psychological qualities for the critical thinking disposition of participants. Results: Average participant scores for critical thinking disposition and mental self-supporting were 280.91 T 28.43 and 76.40 T 8.47, respectively. Positive correlations were observed between these two variables (r = .583, p G .01) and participants’ self-decision, self-cognition, self-confidence, and self-responsibility, which suggest that these factors play a significant role in critical thinking disposition (R2 = .435, p G .01). Conclusions: The participants earned midlevel scores for both disposition toward critical thinking and mental self-supporting abilities. The four factors that had amajor influence on critical thinking disposition included self-decision, self-cognition, self-confidence, and self-responsibility. Nursing educators should focus on improving the critical thinking ability of their students in these four aspects.