Due to their regular and tunable porosity and ultrahigh specific surface area, metal-organic frameworks (MOFs) have been recognized as promising materials for a broad range of applications including: chemical separations, gas storage and release, chemical sensing, catalysis, charge storage, and ionic transport. One of the most attractive characteristics of MOFs is the tunable intra-framework chemical functionality provided by either the spatially well-aligned metal-based nodes or organic linkers. Such intra-framework functional groups may allow the installation of high-density, well-separated, and accessible active sites within the entire frameworksites that are potentially functional for chemical catalysis, photocatalysis, and/or electrocatalysis. Various liquid-and vaporphase post-synthetic methods have been used to attach active moieties to either the linkers or the metal-based nodes of MOFs. For MOF electrochemical applications, a desirable additional property is electrical conductivityan inherently challenging demand, since most MOFs, under most conditions, are electrically insulating. One approach to imparting conductivity is to tether redox-active moieties, such as ferrocene (Fc), to MOF nodes, and then rely upon electron or hole exchange between neighboring neutral and oxidized, or reduced and neutral forms of the tethered species. This mechanism of charge propagation is often termed "redox hopping" and can be contrasted with approaches that instead impart conductivity by introducing band-like electronic properties. It also can be contrasted with approaches that rely upon permeation of MOF channels with a solution containing dissolved redox-active species (for example, methylviologen dications (MV +2 )) that physically shuttle electrons or holes between immobilized electrocatalysts and an underlying electrode. Here we return to the notion of conduction via repetitive charge hopping between MOF tethered/immobilized redox species. We report on our efforts to immobilize ferrocyanide within the mesoporous MOF, NU-1000, and to capitalize on its reversible oxidation to ferricyanide. Perhaps the most widely used redox couple for routine electrochemical studies, apart from ferrocenium/ferrocene and MV 2+/+ , is ferri-/ferrocyanide, i.e. Fe(CN)6 3-/4-.