Abstract
We illustrate with some examples the chemical strategies used to find and optimize the inhibitors of DNA methyltransferases. The knowledge of the structure of the catalytic complexes guides these approaches. The evaluation of the biological activity of the thus designed chemical compounds either confirms the starting hypothesis or brings new elements of structure–activity relationship allowing refinement of the structural hypothesis. In addition, such structure-based strategies enable the proposal of the mechanism of inhibition of the compounds that are then tested experimentally. Perspectives on the optimization will be discussed at the end of the chapter.
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