The Guatemalan moth Tecia solanivora is an invasive pest of potato in Central and South America. The larvae infest potato tubers in the field as well as in storage facilities. The headspace of potato foliage and potato tubers was studied with regard to volatiles that mediate host-finding and oviposition in the Guatemalan moth. Foliage of three phenological stages, from sprouting to tuberization and flowering, released more than 30 sesquiterpenes. The main compounds were beta-caryophyllene, germacrene-D-4-ol, germacrene-D, kunzeaol, and (E,E)-alpha-farnesene. Sesquiterpenes accounted for >90% of the headspace of green plants, whereas fresh potato tubers emitted only trace amounts of a few sesquiterpenes. Screening of headspace collections with antennae of Guatemalan moth females showed a strong response to several sesquiterpenes and monoterpenes that were emitted from foliage only. In addition, antennae responded to methyl phenylacetate, a floral fragrance that was released in large amounts from flowering plants and that was also present in tuber headspace. Female and male moths were attracted to methyl phenylacetate; this compound may accordingly contribute to female attraction to tuber-bearing potato plants in the field as well as to potato tubers in storage. Oviposition tests showed that females lay eggs near mature flowering plants. Eggs were laid in soil close to the plant and not on potato stems and foliage, which may be due to avoidance of terpenoid compounds released from green plant parts at close range. The results support the concept that potato volatiles mediate host-finding and oviposition behavior and that these compounds may become useful tools for management of the Guatemalan moth.