The volatile compounds of crofton weed infested by cotton aphids and sprayed with MeJA were collected and analyzed by the TCT-GC/MS technique. The healthy weeds were controls. Seventeen volatiles identified from crofton weed included green leaf odors, monoterpenes and sequiterpenes, and oxo-compounds. Camphene, 2-carene, α-phellandrene, ρ-cymene, and caryophyllene were the major volatiles and constituted about 77% of the total volatile emissions from the control. In the aphid-infested weeds, no new induced component was found. Among the terpenes, ρ-cymene increased markedly in the infested weeds compared with the control, whereas all sesquiterpenes decreased markedly. Levels of endogenous JA in leaves and young stems of the aphid-infested weeds were markedly higher than in the control, whereas both endogenous SA level and ABA level were not significantly different. MeJA sprayed on crofton weed with the aphid infestation had a similar effect on volatile emissions. It is suggested that JA was one of the most important signals in crofton weed and could regulate the emission of volatile compounds.