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This paper studies the impact of hot pressing on the electrical and thermal performance of thick (thickness >5 μm) conducting polymer poly(3,4-ethylene dioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) films after acid treatment. Thick conducting polymer films usually exhibit low electrical and thermal conductivities similar to bulk polymer because charge and heat carriers are easily scattered by the irregular arrangement of crystalline domains inside the polymer. In this work, the in-plane electrical conductivity of thick hot-pressed PEDOT:PSS film exceeded 1500 S/ cm, and 50% enhancement was obtained in comparison with its nonhot-pressed counterparts. Its in-plane thermal conductivity reached as high as 1.11 W/mK (improved by almost 100% compared to acidtreated PEDOT:PSS films), which is comparable to that of some commercial thermal pads. Such electrical and thermal enhancement via the hot-pressing process is attributed to the optimized morphology and microstructures, which provide short paths for thermal and electrical transportation. We have also demonstrated that the hot-pressed PEDOT:PSS films could be potentially utilized as a flexible conductor and heat spreader for application in flexible electronics and thermal management, respectively. This study not only offers a new insight into the process−property relationship for conducting polymers but also further enables the use of PEDOT:PSS films with simultaneously improved electrical and thermal performance in practical applications, such as thermal management for organic electrodes in batteries, flexible electronics, soft robotics, and bioelectronics.

In this work, we observed size-dependent behavior of filler on both the thermal and electrical conductivities of nacre-like graphene-conjugated conducting polymer films and demonstrated the display of apparent Wiedemann–Franz law and tunability of Lorenz constant in such films. The maximum thermal and electrical conductivities of as-fabricated films can reach over 73 W·m–1·K–1 and 1200 S·cm–1, respectively. Furthermore, the maximum value of electromagnetic interference shielding reaches 54 dB with SSE/t over 16000 dB·cm2·g–1. These films can not only show high-quality electromagnetic interference shielding performance with small thickness and low filler ratio but also achieve simultaneous thermal management during electromagnetic shielding. The findings in this work offer new insight into designing flexible graphene-conjugated polymers with customizable thermal and electrical properties in the broad fields of thermal management systems, electromagnetic defense systems, and flexible electronic systems.