This research studied 31 volatile compounds for indoor control of the medically important mosquitoes Aedes aegypti L. and Culex quinquefasciatus Say. Only adult female mosquitoes were tested. The test compounds were from six families that included five heterobicyclics, eight formate esters, formic acid (a hydrolyzed metabolite of formate esters), eight acetate esters, four propionate esters, three butyrate esters, and two valerate esters. Also, the organophosphate compound dichlorvos (DDVP) was tested as a positive control. Cx. quinquefasciatus was generally more susceptible than Ae. aegypti. Cx. quinquefasciatus was most susceptible to a subset of heterobicyclics and formate esters (rank: n-butyl formate > hexyl formate = dihydrobenzofuran = menthofuran = heptyl formate = ethyl formate). Ae. aegypti was most susceptible to a subset of formate esters (rank: methyl > n-butyl > propyl = ethyl = hexyl). The most active materials against both species had LC₅₀s of 0.4–1 mg active ingredient per 0.5 liter of air volume (0.8–2 mg/liter), which is 50- to 60-fold less toxic than dichlorvos (an organophosphate insecticide that is being phased out from indoor use). In relation to Drosophila melanogaster Meigen, both mosquito species were generally more susceptible to formate esters but more tolerant of heterobicyclics. Generally, the most toxic compound against all dipterans tested to date is n-butyl formate, whereas menthofuran is additionally toxic against Cx. quinquefasciatus and D. melanogaster. Finally, the toxicity differences between species point to the potential for differential toxicity among mosquito genera/species, suggesting that further studies of a number of mosquito species might be warranted.