The sweetpotato weevil (SPW) [Cylas formicarius elegantulus (Summers) (Coleoptera: Curculionidae)] is the single most devastating pest of the sweetpotato [Ipomoea batatas (L.) Lam.] worldwide. Attempts to develop host-plant resistance have been only moderately successful due in part to deficiencies in parent and progeny selection methods. Host-plant phytochemicals play critical roles in insect behavior, modulating a cross-section of key behavioral decisions. Thus, identification of the phytochemicals the female weevil uses in decision making could greatly facilitate development of host-plant resistance. The volatile chemistry of the sweetpotato was studied in relation to the host-finding behavior of the female weevil. Critical biologically active volatiles were determined via isolation (Tenax trapping), fractionation (gas chromatography-thermal conductivity detector), identification (gas chromatography and gas chromatography-mass spectroscopy), and bioassay (olfactometry). Differences in volatile chemistry among sweetpotato clones that may relate to differences in resistance or susceptibility to the female SPW were assessed. Volatile extracts from storage roots (site of oviposition) and aerial plant parts were attractive to female SPW, the former being substantially greater. In total, 33 compounds were identified from storage roots and aerial plant parts, including 23 terpenes. Three oxygenated monoterpenes (nerol, Z-citral, and methyl geranate), found in storage roots but not aerial plant parts, were identified as attractants. The sesquiterpene volatile fraction was repellent to female SPW with α-gurjunene, α-humulene, and ylangene active in the concentration range emanating from storage roots. The aerial plant parts emanated a higher composite concentration of sesquiterpenes than storage roots. Differences in the relative attraction among four sweetpotato cultivars to female SPW was inversely correlated with the composite concentration of headspace sesquiterpenes. Selection of clones with decreased volatile attractants and/or increased deterrents using an analytical means of quantification may significantly facilitate developing resistance to the SPW.