Although rapid electron transfer to HGC-bound molecules has been demonstrated, to the best of our knowledge there have been no reports on using this approach to bind molecular catalysts to electrode surfaces, likely because the dynamic HGC formation in solution phase suggests that rapid desorption would occur. We demonstrate, however, that molecular guests bind with surprisingly high stability and show that these are catalytically active. We also show that the binding of the guests is reversible under controlled conditions and exchange of these guests can be induced. We further demonstrate regeneration of the catalytic activity of the electrodes after re-adsorption of fresh electrocatalytic guests, implying the high stability of the host under operational conditions of the bound catalysts.