Tribulus terrestris L. (TT) (puncturevine) is a common weed that grows in many countries worldwide and in some places is considered as a noxious weed. The plant has been used in traditional Chinese and Indian medicines and is now considered as one of the most popular aphrodisiacs. It is known for its healing properties for sexual difficulties, impotence, and human and animal hormonal imbalance. It is also used as a sexual booster. Because of the plant’s active substances that can be used for curing sexual and other disorders, interest in it is increasing, and it is currently one of the most studied medicinal plants. The products and preparations manufactured from the aboveground plant parts are especially popular among athletes and people with health issues and diseases such as hormonal imbalance, sexual problems, heart problems, and various kidney and skin diseases. The aim of this review is a comprehensive and critical assessment of the scientific publications involving TT, with special reference to its chemical constituents and biological properties that may facilitate current understanding and future studies of this fascinating plant species. The objectives of this review were (1) to find knowledge gaps, (2) to discuss critically relevant publications and issues with materials and methods that may be prerequisites for contradictory results, and (3) to identify research and development areas. It was found that some of the studies on TT extracts as aphrodisiacs are controversial. A significant number of research publications claim that TT extracts and nutritional supplements containing TT improve muscle tone, have a common biostimulating effect, and improve spermogenesis. However, there are a growing number of publications that dispute these claims, as there are no empirical data on commonly accepted mechanisms of action. The main biologically active substances in TT are steroidal saponins, flavonoids, alkaloids, and lignan amides, the most studied being the steroidal saponins. Multiyear data on the metabolic profile of the species are generally lacking. There are a variety of methods used for extracting plant material, differences in methodologies and saponin analyses, and scientific instruments that were used. Lack of common standards could be a reason for differences in the pharmacological activity and composition of the TT preparations. Development of standard procedures and methods for collection of plant material and analyses are recommended. Selection and breeding efforts and agronomic studies of promising clones of TT would need to be conducted in order to develop TT as a new crop. This will provide consistency of supply and quality of the feedstock for the pharmaceutical industry and could provide a new cash crop for growers.