Dietary changes affect the composition and structure of gut microbiota (GM) in animals and humans. One of the beneficial effects of consuming products derived from plants is the positive influence on immunity and gastrointestinal health. Species belonging to the genus Allium contain many organosulfur compounds (OSCs) that have been widely studied showing their biological properties and beneficial effects on intestinal health and GM. This is the first systematic review of OSCs from Allium performed following the Preferred Reporting Items for Systematic Reviews and Meta-Analyses (PRISMA) guidelines, and it is based on the evidence that we found in literature about the benefits on the GM and intestinal health demonstrated by OSCs from Allium, and specifically from onion. OSCs from Allium cepa have shown a significant antibacterial activity against a broad spectrum of antibiotic-resistant Gram-positive and Gram-negative bacteria. In addition, the intake of OSCs from onion was able to modulate the composition of GM, increasing the beneficial bacterial populations in animal models. Moreover, the beneficial effects observed in murine models of colitis suggest that these compounds could be suitable candidates for the treatment of inflammatory bowel disease (IBD) or reverse the dysbiosis caused by a high-fat diet (HFD). Despite the evidence found both in vitro and in vivo, we have not found any article that tested OSCs different from allicin in clinical trials or dietary intervention studies in humans. In this sense, it would be interesting to conduct new research that tests the benefits of these compounds in human GM.