Background: This study aims to investigate the effect of two interventions (verbal advice and comic books) on health literacy and medication compliance among older adults living in 15 public estates in Hong Kong. Methods: This is a two-phase multi-site quasi-experimental study with a pre-and-post design with four measurement points (T1–T4). In both phases, the two interventions were conducted by trained medical/nursing/pharmacy students. Two home visits were carried out in each phase. After the baseline measurement at Time 1 (T1), students verbally advised the older adult participants on how to read, understand, and interpret information on drug labels and how to store drugs properly. A post-assessment was conducted at T2. One year later, another pre-assessment was conducted at T3, and then students used a comic book to educate the older adults. A post-assessment was carried out at T4 after the use of the comic book. Health literacy was measured using the 24-item Chinese Health Literacy Scale for Chronic Care and medication compliance was measured using the Medication Compliance, Knowledge and Storage scale. Generalised Linear Mixed Models were used. Results: A total of 165 subjects were included. The majority (60.6%) were female, aged from 67 to 96. About half (47.3%) had received no formal education. Controlling for age and cognition, there was a significant increase in health literacy after the use of the comic book (coefficient = 2.742, p = 0.001). There was also a significant improvement in medication compliance (total score) (coefficient = −1.018, p < 0.001), reduced knowledge deficiency (coefficient = −0.236, p < 0.05), and reduced storage problems (coefficient = −0.293, p = 0.001) after using comic books. Conclusion: Comic books are a good strategy to improve the health literacy level and medication compliance of community-dwelling older adults.