The purpose of this study was to evaluate the effectiveness of Web-based animated pedagogical agents on critical thinking among nursing students. A pedagogical agent or virtual character provides a possible innovative tool for critical thinking through active engagement of students by asking questions and providing feedback about a series of nursing case studies. This mixed methods experimental study used a pretest, posttest design with a control group. ANCOVA demonstrated no significant difference between the groups on the Critical Thinking Process Test. Pre- and post-think-alouds were analyzed using a rating tool and rubric for the presence of eight cognitive processes, level of critical thinking, and for accuracy of nursing diagnosis, conclusions, and evaluation. Chi-square analyses for each group revealed a significant difference for improvement of the critical thinking level and correct conclusions from pre-think-aloud to post-think-aloud, but only the pedagogical agent group had a significant result for appropriate evaluations.