A novel approach to induce disassembly of electroactive multilayer films fabricated by the layer by layer assembly technique is reported. Electroactive multilayer films are constructed using water soluble polythiophenes, i.e., negatively charged poly[ammonium (3-thienyl)ethoxypropanesulfonate] (SPT) and positively charged poly[3-(3'-thienyloxy)ethyltriethylammonium] (APT). "Induced" dissolution of the films in response to applied potential is investigated using a quartz crystal microbalance equipped with an electrochemical cell module (EC-QCM-D). Disassembly of the films is observed in response to three different potentials: +650, -650, and ±650 mV; however the time for dissolution varies as a function of the potential with films subject to +650 mV dissolving fully in 19 h compared to 42 h for films subject to -650 mV. These electroactive films and their controlled dissolution under applied potential represent an attractive architectural feature for bionic devices that could benefit from their conductivity and dissolution over time. © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.