With the development of smart delivery systems for pesticides, many studies revealed that nanodelivery methods have great potential for use in efficient and sustainable agriculture; however, field application of the nanopesticides is still a challenge. In this study, the application of a chlorfenapyr (CF)-loaded iron-based metal–organic framework (CF@MIL-101-SL) to maize and its control efficacy for Spodoptera frugiperda were investigated in detail. The results showed that, compared with a suspension concentrate of CF (CF-SC), a solution of CF@MIL-101-SL with the surfactant aerosol OT exhibited excellent wetting, deposition and adhesion with maize leaves. The CF@MIL-101-SL NPs exhibited bidirectional translocation in maize, which significantly enhanced the transport of CF to the target tissues. Field trials revealed that CF@MIL-101-SL maintained > 75 % control efficiency after 21 d of spraying, indicating significantly greater insecticidal activity and persistence than CF-SC. Spray application of CF@MIL-101-SL gave high initial deposition rates, long half-lives on tender and old leaves and significantly reduced pesticide drift into the environment. Based on a biosafety assessment, spraying with CF@MIL-101-SL reduced the negative effects of CF on plants during the growth period. In addition, CF@MIL-101-SL increased the survival rate of Harmonia axyridis larvae and reduced the impacts of CF on the growth and intestinal damage of Harmonia axyridis. In summary, these results highlight the advantages of metal–organic framework delivery systems for multidimensional enhancement of pesticide efficacy, persistence, and safety and provide data on field application and the environmental risks of nanodelivery systems.