A new series of 1, 5-disubstituted 1, 3, 5-hexahydrotriazine-2-N-nitroimines (4a–4x) were designed and synthesized as novel chiral neonicotinoid analogues. The single-crystal structure of 4n was further determined by X-ray diffraction, and its S configuration was confirmed. Preliminary bioassay showed that compound 4e, 4k, 4u, 4v exhibited excellent insecticidal activities at 100 mg/L, while 4k had> 90% mortality at 10 mg/L, which ...