This study developed smartphone-based virtual experiential nursing applications to care for patients with chronic illness, especially patients with hypertension and diabetes, and evaluated the effect of the applications on nursing students’ knowledge, self-efficacy, and learning experiences. Applications using gamification elements were developed according to the steps of assessment, design, development, implementation, and evaluation. Knowledge and self-efficacy were assessed via questionnaires, while learning experiences were assessed via six focus group interviews after the applications were used for 1 week. Quantitative data were analyzed using descriptive analysis, χ2 test, Fisher’s exact test, t test for the homogeneity of participants (experimental, 49; control, 43), an independent t test, and a paired t test for effectiveness in each group. Qualitative data were analyzed using qualitative thematic analysis. Knowledge on hypertension (t = 4.41, P < .001) and diabetes (t = 2.45, P < .009), as well as self-efficacy for hypertension (t = 3.08, P < .002) and diabetes (t = 1.75, P < .043), significantly improved in the experimental group compared to the control group. Students may use the applications as complementary learning resources without the limitations of time and space, and students were satisfied overall with their use. The chronic illness care smartphone applications are effective learning resources that assist students in assessing patients’ health problems and implementing nursing care plans to improve patient conditions.