Synthetic chemistry for molecular imprinting is a necessary ‘jack-of-all-trades’ no matter what application the molecularly imprinted polymers (MIPs) aim for. There is significant interest in developing different types of chemistry for MIPs so that these can be used as selective materials towards analyte sensing. Therefore, this chapter discusses the comprehensive approaches to syntheses of MIPs, including design of functional monomers providing different types of interactions with templates, imprinting and polymerization techniques to form templated MIPs, and template removal. The versatile usage of MIPs as the selectively sensing materials for a broad range of analytes from macro-sized cells, viruses, bacteria, to sub-nano-sized metal ions and organic contaminants is then demonstrated.