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Two different interlayer structured glyphosate (GLY) intercalated MgAl layered double hydroxides, as novel pesticide slow/controlled release materials, have been synthesized by co-precipitation method under various reaction pH values. The slow/controlled release properties have been tested in Na2CO3 aqueous solution. The release mechanism has been interpreted on the basis of the ion-exchange between the guest GLY anions in the lamellar host and in the release media, and the diffusion process of GLY anions in the interstice and interlayer of GLY intercalates, i.e. diffusion through the particles, is the rate-limiting step of GLY release process. The GLY intercalate assembled at lower pH, possessing higher interlayer gallery height and vertical monolayered arrangement of guest anions in the interlayer with larger packing density, exhibits better slow release property than that assembled at higher pH. The results reveal that the layered double hydroxides have potential application in the pesticide slow/controlled release area.