Mixed protonic-electronic conductors (MPECs) have been developed to maximize static conductivity for electrochemical applications, but emerging applications that leverage proton-electron coupling (PEC) require dynamic conductivity control. To achieve this, we propose a "de-doping" strategy in a hydrogen-bonded coordination polymer {Co(DMF)2(H2O)2(bipy)2·2(DMF)}n (bipy = 4,4'-bipyridine, DMF = N,N-dimethylformamide) named Co