The reversible interconversion of protons and dihydrogen is an electrochemical process of fundamental importance to a hydrogen economy. The process requires catalysis to proceed at practical rates at moderate temperatures. Currently platinum is the preferred electrocatalyst in reversible hydrogen fuel cells. The supply of this metal is limited and in the long term unsustainable. The metal-sulfur catalytic sites of hydrogenases are built from abundant elements and catalyse hydrogen evolution or uptake at rapid rates. Mechanistic studies of the hydrogenases of synthetic assemblies and of in silico models is driven, at least in part, by the view that understanding active-site structure and function will inform the design of new materials for hydrogen production or uptake]. We have shown that iron-sulfur cluster analogues of the electron-transfer centres in the {4Fe4S}-ferredoxin redox proteins can be built into cysteinyl functionalised poly(pyrroles) and that such arrays sustain fast charge propagation through an electrode-bound polymer film. Incorporating synthetic analogues of the catalytic machinery of iron-only hydrogenase within an electropolymer presents a greater challenge, but one which might afford new electrode materials for electrocatalysis of dihydrogen uptake/evolution. This is particularly attractive if catalysis can be matched to the conducting regime of the supporting polymer or fast electron-transfer relays are co-incorporated.  Some first steps in this direction have now been taken:  the assembly of solid-state materials with structures related to the subsite and H-cluster of iron-only hydrogenase confined within an electropolymer framework.