The purposes of this study are threefold: 1) to find out what characteristics are required for the successful use of ePortfolios; 2) to discover what activities best represent reflective thinking during the use of ePortfolios; and, 3) to investigate the interrelationship between nursing staff users' perceived success levels with ePortfolios and with their reflective thinking activities. Survey methodology was used to gather responses from 78 nurses from a medical center located in southern Taiwan via questionnaires. Factor analysis and canonical correlation analysis were used to analyze the collected data. The results demonstrated that system quality, information quality, and user satisfaction are important variables in successful ePortfolio usage; while habitual action, understanding, reflection, and critical reflection are major variables of reflective thinking. Further, we found a significant relationship exists between the relative success of ePortfolios and reflective thinking activities of ePortfolios users. The subject hospital should pay special attention to important characteristics including system quality, information quality, and user satisfaction when employing ePortfolios to help nursing staff users to achieve their learning goals through this form of reflective thinking.