Aflatoxins (AFs) are secondary metabolites produced by Aspergillus spp., known for their hepatotoxic, carcinogenic, and mutagenic activity in humans and animals. AF contamination of staple food commodities is a global concern due to their toxicity and the economic losses they cause. Different strategies have been applied to reduce fungal contamination and AF production. Among them, the use of natural, plant-derived compounds is emerging as a promising strategy to be applied to control both Aspergillus spoilage and AF contamination in food and feed commodities in an integrated pre-and postharvest management. In particular, phenols, aldehydes, and terpenes extracted from medicinal plants, spices, or fruits have been studied in depth. They can be easily extracted, they are generally recognized as safe (GRAS), and they are foodgrade and act through a wide variety of mechanisms. This review investigated the main compounds with antifungal and anti-aflatoxigenic activity, also elucidating their physiological role and the different modes of action and synergies. Plant bioactive compounds are shown to be effective in modulating Aspergillus spp. contamination and AF production both in vitro and in vivo. Therefore, their application in pre-and postharvest management could represent an important tool to control aflatoxigenic fungi and to reduce AF contamination.