Apiaceae L. contains many potential plants as repellent and insecticidal resources. However, Ligusticum applied in the stored insect control is still under-evaluated. Hence, the chemical composition and bioactivities of five Ligusticum plants with abundant resources were investigated in this study against Tribolium castaneum (Coleoptera: Tenebrionidae), Lasioderma serricorne (Coleoptera: Anobiidae), and Liposcelis bostrychophila (Psocoptera: Liposcelididae). The contact toxicity was found 24 h after treatment with Ligusticum pteridophyllum, Ligusticum ajanense, Ligusticum chuanxiong, Ligusticum thomsonii, and Ligusticum jeholense essential oils (LD50 = 87.99, 44.01, 21.53, 125.37, and >50% mu g/adult; 89.82, 93.51, 28.42, 105.55, and 50.16 mu g/adult; 7.87, 308.62, 67.82, and 195.06 mu g/cm(2), respectively). The five plants' essential oils possessed poor fumigant toxicity against three target insects at the highest concentration. Moreover, all analyzed oils have good repellent activity in a dose-dependent manner. In conclusion, the tested oils have the potential to be developed as contact and repellent agents in protecting the stored products.