(1) Background: Virtual reality (VR) technology is a widely used training tool in medical education. The present study aimed to evaluate the effectiveness of VR training of oral hygiene students on providing oral healthcare to disabled elderly persons. (2) Methods: A randomized controlled trial was conducted. In 2021, oral hygiene students were randomly assigned to a VR experimental group (EG; n = 11) and a control group (CG; n = 12). The EG received two-hour, thrice-repeated VR-based training interventions at 2-week, 4-week, and 6-week follow-ups. The CG received no VR-based interventions. Data were collected using a self-administered questionnaire before and immediately after each intervention. We performed generalized estimating equations to compare the responses. (3) Results: The EG exhibited a more significant improvement in oral care-related knowledge, attitude, self-efficacy, and intention at the 6-week follow-up than the CG. The students’ intention to assist the elderly in using interdental brushes (β = 0.91), with soft tissue cleaning (β = 0.53), and with oral desensitization (β = 0.53), and to have regular dental visits (β = 0.61) improved significantly at the 6-week follow-up. (4) Conclusions: VR training positively affected students’ knowledge, attitude, self-efficacy, and intentions on providing oral healthcare to disabled elderly persons.