The current study examined the links between mental health, demographic characteristics, harmful gambling among UK Armed Forces serving personnel (AFSP). A total of 608 currently serving personnel members completed the survey. Most (72%) respondents gambled in the past year. About 23% experienced any level of harmful gambling (PGSI score of 1+). Respondents who were male, aged 20–29 years, and living in service single-living accommodation were more likely to experience any level of harmful gambling. Being a junior non-commissioned officer was the strongest risk factor for problem gambling. Other risk factors included likely experiencing anxiety, engaging in strategic gambling activities, being male, and having suicidal ideas/attempts in the past year. Protective factors included being in a relationship and being a commissioned officer.