Two new chlorinated multiacylated 3,4-seco-grayanane diterpenoids, neopierisoids A and B (1 and 2), were isolated from flowers of the poisonous plant Pieris japonica and were identified from spectroscopic analysis and X-ray diffraction data. Both compounds showed obvious antifeedant activity against Pieris brassicae with an EC50 of 10.07 μg/cm(2) for 1 and 5.33 μg/cm(2) for 2, indications of toxic properties. Chlorinated 3,4-seco-grayanane diterpenoids in P. japonica may play a defensive role against herbivores.