In this study, the impacts of service learning (SL) on the spiritual well-being and psychological health of Chinese university students in Hong Kong are determined. The SL programme is a six-month, credit-bearing programme (not less than 80 working hours). The study adopted a pre-test-post-test quasi-experimental design, wherein students enrolled in SL comprised the experimental group (n = 132; 59 male, 73 female), and those who were not enrolled in SL comprised the control group (n = 128; 55 male, 73 female). The students completed the spiritual well-being questionnaire (SWBQ) to evaluate the status of their spiritual well-being (including the personal and communal, environmental, and transcendental domains), and the Depression, Anxiety and Stress Scale-21 (DASS-21) was used to assess their emotional states of depression, anxiety and stress before and after the SL programme. At pre-test, no significant differences were observed between the two groups in SWBQ and DASS-21 scores. Findings indicated that students in the experimental group had greater increases in spiritual well-being in personal and communal, environmental and transcendental domains and decreases in stress, anxiety and depression than those in the control group at the end of the SL programme.