A multifunctional nanopesticide delivery system is considered to be a novel and efficient tool for controlling pests in modern agriculture. In this study, a mesoporous silica nanosheet (H-MSN) carrier for intelligent delivery of pesticides was prepared by the sol-gel method. The prepared H-MSN carrier had obvious hexagonal flat structure, with a specific surface area of 759.9 m2/g, a transverse diameter of about 340 nm, a thickness of about 80 nm, and regular channels being perpendicular to the plane. Polyethylene glycol diacrylate (PEGDA) and sulfhydryl-modified polyethylenimide (PEI-SH) were used to block the insecticide after loading the insecticide imidacloprid (IMI). The introduction of hydrophilic PEI-SH/PEGDA greatly improved the leaf wettability and adhesion ability of H-MSN. The retention amount of IMI@H-MSN@PEI-SH/PEGDA on cucumber and cabbage leaves was up to 46.0 mg/cm2 and 19.0 mg/cm2, respectively. IMI@H-MSN@PEI-SH/PEGDA showed pH- and GSH-responsive release. Compared with pure IMI, IMI entrapped in MSN carriers has favorable biocompatibility and antiphotolytic properties.