Harmful algal blooms (HABs) have several negative impacts on aquatic ecosystem, and even harm to humans. Utilization of allelochemicals to inhibit microalgal overgrowth is an environment-friendly approach for controlling HABs. This paper demonstrated the development of allelochemicals with algicidal effects, including the development history of allelopathy, the application methods, the reported allelopathic plants and their derived allelochemicals. Allelopathy is a promising strategy to control HABs as the effectiveness of allelochemicals on inhibiting microalgae cells has been discovered and confirmed for many years. The proposed allelopathic mechanisms and species-selective properties were expounded as well. Moreover, this paper further proposed suggestions for the further research and development of allelopathy strategy for HABs control.