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Superelastic graphene aerogel with ultra-high compressibility shows promising potential for compression-tolerant supercapacitor electrode. However, its specific capacitance is too low to meet the practical application. Herein, we deposited polyaniline (PANI) into the superelastic graphene aerogel to improve the capacitance while maintaining the superelasticity. Graphene/PANI aerogel with optimized PANI mass content of 63 wt% shows the improved specific capacitance of 713 F g −1  in the three-electrode system. And the graphene/PANI aerogel presents a high recoverable compressive strain of 90% due to the strong interaction between PANI and graphene. The all-solid-state supercapacitors were assembled to demonstrate the compression-tolerant ability of graphene/PANI electrodes. The gravimetric capacitance of graphene/PANI electrodes reaches 424 F g −1  and retains 96% even at 90% compressive strain. And a volumetric capacitance of 65.5 F cm −3  is achieved, which is much higher than that of other compressible composite electrodes. Furthermore, several compressible supercapacitors can be integrated and connected in series to enhance the overall output voltage, suggesting the potential to meet the practical application.   Electronic supplementary material  The online version of this article (10.1186/s11671-017-2395-z) contains supplementary material, which is available to authorized users.

Graphene/Polyaniline Aerogel with Superelasticity and High Capacitance as Highly Compression-Tolerant Supercapacitor Electrode