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Abstract: A new methodology has been developed to provide effective functionalization of the intersurfaces of ordered, crystalline, layered magadiite via an imprinting synthesis. Although the surface imprinting has been conducted successfully on a variety of substrates, no report has appeared on imprinting synthesis on the intergalleries of the layered materials. This methodology has resulted in a simplified experimental procedure for functionalizing layered silicates with good control of the distributions of functional ligands on magadiite. Our results demonstrate that the imprint-functionalized magadiite has better selectivity and a higher capacity for metal-ion templates than the nonimprinted analogue. The possibility of continuous variation of the basal spacing and the crystalline structures of the layered materials highlight a new opportunity for conducting imprinting synthesis