Nootropics are compounds that enhance cognitive performance and have been highlighted as a medium-term human augmentation technology that could support soldier performance. Given the differing ethical, safety, and legal considerations associated with the pharmaceutical subset of nootropics, this analysis focuses on dietary supplementation which may enhance cognition during training and operations. Numerous supplements have been investigated as possible nootropics, however research is often not context specific or of high quality, leading to questions regarding efficacy. There are many other complex cofactors that may affect the efficacy of any dietary nootropic supplement which is designed to improve cognition, such as external stressors (e.g., sleep deprivation, high physical workloads), task specifics (e.g., cognitive processes required), and other psychological constructs (e.g., placebo/nocebo effect). Moreover, military population considerations, such as prior nutritional knowledge and current supplement consumption (e.g., caffeine), along with other issues such as supplement contamination should be evaluated when considering dietary nootropic use within military populations. However, given the increasing requirement for cognitive capabilities by military personnel to complete role-related tasks, dietary nootropics could be highly beneficial in specific contexts. Whilst current evidence is broadly weak, nutritional nootropic supplements may be of most use to the military end user, during periods of high military specific stress. Currently, caffeine and L-tyrosine are the leading nootropic supplements candidates within the military context. Future military specific research on nootropics should be of high quality and use externally valid methodologies to maximise the translation of research to practice.