Site isolation, compartmentalization and substrate specificity are a few of the characteristics responsible for the catalytic efficiency demonstrated by enzymes in natural systems. In efforts to mimic these highly efficient systems, research has been directed towards macromolecular chemistry. Robust polymer assemblies can create a favorable and isolated environment around the catalytic site allowing specific and sometimes incompatible reactions to take place within this protected reaction pocket. Further exploring the use of ‘smart’ polymers, control over both the catalytic activity and substrate specificity is achieved. In addition, polymeric systems provide the opportunity for recycling of the active catalysts, further enhancing the advantages of polymer supported catalytic systems.