Adult secretions of four Japanese Chrysomelinae, Gastrophysa atrocyanea, Plagiodera versicolora distincta, Chrysomela vigintipunctata costella, and Gastrolina depressa (Coleoptera: Chrysomelidae) were analyzed by TLC, HPLC, NMR and FAB-MS. Three nitropropanoyl isoxazolinone glucosides, 2-[6′-(3″-nitropropanoyl)-β-D-glucopyranosyl]-3-isoxazolin-5-one (1), 2-[2′,6′-di-(3″-nitropropanoyl)-β-D-glucopyranosyl]-3-isoxazolin-5-one (3), and 2-[3′,6′-di-(3″-nitropropanoyl)-β-D-glucopyranosyl]-3-isoxazolin-5-one (4) were found in all species. In addition, two nitropropanoyl glucosides, 1,6-di-(3′-nitropropanoyl)-β-D-glucopyranose (2) and 1,2,6-tri-(3′-nitropropanoyl)-β-D-glucopyranose (5) were also detected from these species. The secretions of the four species and compounds 3 and 5 showed strong deterrent effects against ants (Tetramorium caespitum), whereas compounds 2 and 4 exhibited low activity.