UNLABELLED:Understanding the mechanism of the strain-dependent conductivity change in polymers in stretched conditions is important. We observed a strain-induced growth of the conductive regions of
PEDOT:PSS films, induced by a coalescence of conductive PEDOT-rich cores. This growth due to coalescence leads to a gradual decrease in the electrical resistivity up to 95%, independent of the thickness of the
PEDOT:PSS films. The primary mechanism for the evolution of the PEDOT-rich cores proceeds by the cores growing larger as they consuming relatively smaller cores. This process is caused by a strain-induced local rearrangement of PEDOT segments in the vicinity of PSS shells around the cores and also changes the chemical environment in PEDOT, induced by the electron-withdrawing effects around the PEDOT chains. The strain-induced growth mechanism is beneficial to understanding the phenomenon of polymeric chain rearrangement in mechanical deformation and to modulating the electrical conductivity for practical applications.