Dental hygiene students find it challenging to understand and perform the dental hygiene process of care (DHPC) after only a limited amount of clinical training; they generally improve their DHPC skills through clinical experience after graduation. In this study, we developed and evaluated interactive learning materials that simulate the DHPC. We divided the learning contents of the DHPC into six components and created five simulation materials. Using these materials, students could experience a typical DHPC virtually. In total, 30 third-year university dental hygiene students were divided into two groups (A and B), and then pre-quizzes were carried out for each group (group A: Quiz I, group B: Quiz II). Next, the students learned using the developed materials and took post-quizzes (group A: Quiz II, group B: Quiz I) to clarify their understanding of the DHPC. After the post-quizzes, a questionnaire survey was conducted. Both groups showed significantly higher scores on the post-quiz than on the pre-quiz (Group A: p = 0.0451 vs. Group B: p = 0.0090, paired Student’s t-test). In addition, more than 80% of the responses to the questionnaire were favorable. These results suggest that the simulation materials developed in this study are effective for learning the DHPC