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Abstract: Molecular-imprinting technology is now firmly established as a way of preparing polymers with specifically shaped cavities for the recognition of small molecule templates. The use of emulsion polymerisation to form core-shell particles (CS-MIPs), whereby the imprinting occurs at the surface of a polymer colloid (ca.100 nm diameter), has been shown to be a very effective way of creating open-faced cavities for the recogntion of shape and functionality in molecules such as caffeine and its analogue theophylline. It was confirmed by the use of a 14C-labelled caffeine radiotracer study, using liquid scintillation counting, that removal of 100% of the template caffeine can be carried out using mild solvent extraction procedures. Binding studies were also carried out to probe the surface molecular imprinting effect and Scratchard analysis gave a biphasic binding curve for the binding of caffeine to a caffeine-imprinted CS-MIP.