摘要： We demonstrate controlled charge trapping and release, accompanied by multiple color changes in a metallo-organic bilayer. The dual functionality of the metallo-organic materials provides a fundamental insight into the metal-mediated electron transport pathways. The electrochemical processes are accompanied by distinct, four color–to–color transitions: red, transparent, orange, and brown. The bilayer consists of two elements: (i) a nanoscale gate consisting of a layer of well-defined polypyridyl ruthenium complexes bound to a flexible transparent electrode, and (ii) a charge storage layer consisting of isostructural iron complexes attached to the surface of the gate. This gate mediates or blocks electron transport in response to a voltage. The charge storage and release depend on the oxidation state of the layer of ruthenium complexes (= gate). Combining electrochemistry with optical data revealed mechanistic information: the brown coloration of the bilayer directly relates to the formation of intermediate ruthenium species, providing evidence for catalytic positive charge release mediated through the gate.