The hot‐stretching method has been well accepted for enhancing the electrical conductivity of conducting polymer films. High temperature is the prerequisite to soften the polymer to highly align and elongate the polymeric molecular chains. In this study, the cold‐stretching method is proposed for the first time to enhance the conductivity of conducting polymeric films. Polyaniline (PANI) films are stretched at room temperature to different strain levels. It is observed that the applied strain has significant effects on the morphology, molecular chain structure, crystallinity, and crosslinking of the PANI films. As a result, the conductivity of PANI films is effectively increased by the cold‐stretching process. Particularly, a maximum conductivity with an 18.4‐fold increase in the direction parallel to the stretched direction is obtained when the elastic limit strain is applied. Compared to hot stretching, cold stretching is unique due to the extremely low dimensional change and very high efficiency achieved.magnified image

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