The use of pesticides together with nano-delivery systems can improve the utilization rate of pesticides due to the envelope and controlled release function of nano-carriers. This precisely matches the needs of different target crops. Herein, a dinotefuran supramolecularly bonded layered double hydroxide (D-LDH) nano-pesticide has been designed to improve the controlled release properties and insecticidal activity in cucumber and cotton plants. As confirmed by XRD patterns, FT-IR spectroscopy, SEM images and zeta potentials, dinotefuran molecules are supramolecularly bonded onto LDH nano-carriers, which can be effectively controlled by regulating the carrier ratio. The wettability performance and foliar surface adhesion of D-LDH are significantly improved due to hydrogen bonding interaction. The control effect of D-LDH on Aphis gossypii remains 90.1% after 60 days, which means only a one time application can achieve effective control during the whole growth cycle. The applications of foliar spraying on cucumber against Trialeurodes vaporariorum and Bemisia tabaci show that the control effect is still more than 80% after 14 days when the dose is ∼33% less than the recommended minimum dose. Overall, this novel D-LDH nano-pesticide shows the possibility in improving the utilization rate of pesticides and reducing application times.