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This paper describes a non‐invasive approach for efficient detachment of cells adhered to a gold substrate via a specific oligopeptide. Detachment is effected by an electrical stimulus. The oligopeptide contains cysteine, which spontaneously forms a gold–thiolate bond on a gold surface. This chemical adsorption reaches > 95% equilibrium within 10 min after immersion of a gold‐coated substrate in a solution containing the peptide. The peptide is reversibly desorbed from the surface within 5 min of application of a negative electrical potential. By taking advantage of this simple adsorption and desorption mechanism, cells can be grown on an oligopeptide‐functionalized gold surface and can be efficiently detached as single cells or cell sheets by application of a negative electrical potential. This approach was also applied to the surface of gold‐coated microrods. Capillary‐like microchannels were formed in …