Cyanobacterial harmful algal blooms (Cyano-HABs) are an international environmental problem that negatively affects the ecosystem as well as the safety of water resources by discharging cyanotoxins. In particular, the discharge of microcystins (MCs), a highly toxic substance, has been studied most actively, and various water treatment methods have been proposed for this purpose. In this paper, we reviewed adsorption technology, which is recognized as the most feasible, economical, and efficient method among suggested treatment methods for removing MCs. Activated carbons (AC) are widely used adsorbents for MCs removal, and excellent MCs adsorption performance has been reported. Research on alternative adsorption materials for AC such as biochar and biosorbents has been conducted, however, their performance was lower compared to activated carbon. The impacts of adsorbent properties (characteristics of pore surface chemistry) and environmental factors (solution pH, temperature, natural organic matter, and ionic strength) on the MCs adsorption performance were also discussed. In addition, toward effective control of MCs, the possibility of the direct removal of harmful cyanobacteria as well as the removal of dissolved MCs using adsorption strategy was examined. However, to fully utilize the adsorption for the removal of MCs, the application and optimization under actual environmental conditions are still required, thereby meeting the environmental and economic standards. From this study, crucial insights could be provided for the development and selection of effective adsorbent and subsequent adsorption processes for the removal of MCs from water resources.