The pursuit of intelligent optoelectronics could have profound implications on our future daily life. Simultaneous enhancement of the electrical performance, mechanical stretchability, and optical transparency of semiconducting polymers may significantly broaden the spectrum of realizable applications for these materials in future intelligent optoelectronics, i.e., wearable devices, electronic skin, stretchable displays, and a vast array of biomedical sensors. Here, semiconducting films with significantly improved mechanical elasticity and optical transparency, without affecting the film’s electronic conductivity even under 100% strain, were prepared by blending only a small amount (below 1 wt %) of either p-type or n-type commercial semiconductor polymers. We demonstrate that a self-organized versatile conjugated polymer film displaying an interpenetrating polymer network is formed in the semiconducting films and is crucial for the observed enhancement of elasticity, optical transparency, and charge-carrier mobility. On the basis of this versatile semiconducting film, we explored a new practical approach to directly integrate all the stretchable components for a large area transistor array through solution processing and a final single, mechanical peel-off step. We demonstrate robust transistor arrays exhibiting charge carrier mobilities above 1.0 cm2/V s with excellent durability, even under 100% strain. We believe our achievements will have great impact on stretchable optoelectronic devices for practical applications and represent promising directions for industry-scale production of stretchable displays and wearable electronic devices.

Although stretchable polymer-based devices with promising electrical performance have been produced through the polymer blend strategy, the interplay between the blend film microstructure and macroscopic device performance under deformation has yet to be unambiguously articulated. Here, we discuss the formation of robust semiconducting networks in blended films through a thermodynamic perspective. Thermodynamic behavior along with the linear absorption and photoluminescence measurements predict the competition between polymer phase separation and semiconductor crystallization processes during film formation. Semiconducting films comprised of different pi-conjugated semiconductors were prepared and shown to have mechanical and electronic properties similar to those of films comprised of a model P3HT and PDMS blend. These results suggest that a film’s microstructure and therefore robustness can be refined by controlling the phase separation and crystallization behavior during film solidification. Fine-tuning a film’s electrical, mechanical, and optical properties during fabrication will allow for advanced next-generation of optoelectronic devices.

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