Electrocatalytic [FeFe]-hydrogenase mimics for the hydrogen evolution reaction (HER) generally suffer from low activity,h igh overpotential, aggregation, oxygen sensitivity, and low solubility in water.B yu sing atom-transfer radical polymerization (ATRP), an ew class of [FeFe]-metallopolymers with precise molar mass,d efined composition, and low polydispersity,h as been prepared. The synthetic methodology introduced here allows facile variation of polymer composition to optimize the [FeFe] solubility,a ctivity,a nd long-term chemical and aerobic stability.W ater soluble functional metallopolymers facilitate electrocatalytic hydrogen production in neutral water with loadings as low as 2ppm and operate at rates an order of magnitude faster than hydrogenases (2.5 10 5 s À1 ), and with lowoverpotential requirement. Furthermore, unlike the hydrogenases,these systems are insensitive to oxygen during catalysis,with turnover numbers on the order of 40 000 under both anaerobic and aerobic conditions.