Several 6-aryl-9-benzylpurines have been shown to be selective antagonists for various adenosine receptors including A1, A2A, A2B and A3. The structures of the most active compounds resemble those screened in the Mycobacterium tuberculosis (Mtb) project in our group. Some of these compounds were also screened for the adenosine receptors. The results from this screening and the exploration of structure-activity relationship (SAR) made the foundation for synthesizing new purine analogous as selective adenosine receptor antagonist. The target compounds were successfully synthesized with Stille and Suzuki coupling reactions and new effective methods have been developed. Herein the chemistry will be discussed.