Around the world, mosquitoes continue to transmit disease-causing pathogens and develop 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 5 more chemically related compounds for mosquito lethality and 8 GRAS sugar substitutes to determine toxicity. 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 (Diptera, Culicidae, Linnaeus, 1762) and Aedes albopictus (Diptera, Culicidae, 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 h. We also found that there were different responses in the 2 species and that in several experimental conditions, male mosquitoes expired to a greater extent than female mosquitoes. These findings indicate that several of the compounds are toxic to mosquitoes. Further study is required to determine their effectiveness in attractive toxic sugar baits (ATSBs) as a potential component of population control strategies.