The global expansion of harmful cyanobacterial blooms (CyanoHABs) poses an increasing threat to public health. CyanoHABs are characterized by the production of toxic metabolites known as cyanotoxins. Human exposure to cyanotoxins is challenging to forecast, and perhaps the least understood exposure route is via inhalation. While the aerosolization of toxins from marine harmful algal blooms (HABs) has been well documented, the aerosolization of cyanotoxins in freshwater systems remains understudied. In recent years, spray aerosol (SA) produced in the airshed of the Laurentian Great Lakes (United States and Canada) has been characterized, suggesting that freshwater systems may impact atmospheric aerosol loading more than previously understood. Therefore, further investigation regarding the impact of CyanoHABs on human respiratory health is warranted. This review examines current research on the incorporation of cyanobacterial cells and cyanotoxins into SA of aquatic ecosystems which experience HABs. We present an overview of cyanotoxin fate in the environment, biological incorporation into SA, existing data on cyanotoxins in SA, relevant collection methods, and adverse health outcomes associated with cyanotoxin inhalation.