Around the world, mosquitoes continue to transmit disease-causing pathogens while also developing resistance to insecticides. We previously discovered that a generally regarded as safe (GRAS) compound, 1,2-propanediol, reduces adult mosquito survivorship when ingested. In this study, we assess and compare five more chemically related compounds for mosquito lethality and eight GRAS sugar substitutes to determine toxic effects. We conducted a series of feeding assays to determine if ingesting the compounds influenced mosquito mean survivorship in locally collected lab-reared populations of Aedes aegypti (Linnaeus, 1762) and Aedes albopictus (Skuse, 1894) mosquitoes. Our results indicate that 1,2-propanediol, 1,3-propanediol, 1,5-pentanediol, 1,6-hexanediol, 2-methyl-1,3-propanediol, DL-dithiothreitol, acesulfame potassium, allulose, erythritol, sodium saccharin, stevia, and sucralose significantly reduced the mean survivorship of one or both species. Short-term trials with the most toxic compounds revealed that they could substantially affect survivorship after 24 hours. We also found that many of the compounds yielded different responses in the two species and that male mosquitoes expired to a greater extent than female mosquitoes. These findings indicate that several of the compounds may be highly effective for local mosquito vector population and disease control through functioning as components in attractive toxic sugar bait systems (ATSBs)