Dietary supplements (DSs) and nutritional supplements (NSs) can enhance performance, recovery or training adaptations, however, some substances, dosages, and usage protocols are unsafe. Knowledge of the type and extent of use within populations enables strategies to be formulated to promote safe and effective use (where needed) and to avoid adverse side effects. The purpose of this study was to understand DS and NS use by active-duty Australian soldiers. Surveys were distributed by e-mail and hard copy to eligible participants (n = 23,195). Respondents (males n = 1833; females n = 296) comprised 9.3% of the total population. Use of ≥1 DSs/week was reported by 76.4% of males and 86.8% of females, and use of ≥1 NSs/week was reported by 21.7% of males and 20.9% of females. The most commonly used supplements were protein or amino acids (55.6%), multivitamins and minerals (38.2%), other DSs (37.8%), individual vitamins and minerals (33.0%), and combination products (32.8%). Logistic regression revealed the number of DSs respondents used simultaneously was significantly different between males and females, age groups, BMI ranges, and body weight actions. Engagement in special operations was a significant predictor of the use of any DS, individual vitamin and minerals and multivitamin and minerals. Approximately 16% of regular DS users reported experiencing one or more side effects, with the most common being palpitations (10.6%), tingling or numbness in the face, fingers, arms, or legs (5.5%), tremors or shaking (2.9%), flushing (2.3%), headache (2.0%), abdominal pain (1.6%), anxiety (1.4%), and dizziness or confusion (0.9%). The results revealed more prevalent use of several categories of DSs and NSs among some subgroups. Ongoing surveillance of DS and NS use is important for tracking trends in use over time and gauging the effectiveness of any strategies employed to enhance the quality of supplement use.