Aedes aegypti and Anopheles gambiae are two mosquito species that represent significant threats to global public health as vectors of Dengue virus and malaria parasites, respectively. Although mosquito populations have been effectively controlled through the use of synthetic insecticides, the emergence of widespread insecticide-resistance in wild mosquito populations is a strong motivation to explore new insecticidal chemistries. For these studies, Ae. aegypti and An. gambiae were treated with commercially available plant essential oils via topical application. The relative toxicity of each essential oil was determined, as measured by the 24-h LD50 and percentage knockdown at 1 h, as compared with a variety of synthetic pyrethroids. For Ae. aegypti, the most toxic essential oil (patchouli oil) was ∼1,700-times less toxic than the least toxic synthetic pyrethroid, bifenthrin. For An. gambiae, the most toxic essential oil (patchouli oil) was ∼685-times less toxic than the least toxic synthetic pyrethroid. A wide variety of toxicities were observed among the essential oils screened. Also, plant essential oils were analyzed via gas chromatography/mass spectrometry (GC/MS) to identify the major components in each of the samples screened in this study. While the toxicities of these plant essential oils were demonstrated to be lower than those of the synthetic pyrethroids tested, the large amount of GC/MS data and bioactivity data for each essential oil presented in this study will serve as a valuable resource for future studies exploring the insecticidal quality of plant essential oils.