LAUSR

Ionic liquids (ILs) or solidified ionic liquids, known as ionogels, have been actively employed in supercapacitors (SCs) owing to their superior electrochemical stabilities to aqueous and organic electrolytes. However, initial efforts of using ILs and ionogels in SCs were not successful because bulky and sluggish ions cannot effectively access tiny pores of conventional microporous carbons. To address this, a strategy is developed to optimize the electrochemically active surfaces of carbonaceous electrodes and thus to improve the energy storage performance by incorporating 3D ordered/interconnected large mesoporous carbons with ionogel electrolytes. Precisely designed large mesopores interconnected via windows promote mass transport of the electrolyte ions within the solid ionogel electrolytes and effectively utilize the surface of the carbon electrodes for capacitive energy storage, giving rise to record‐high energy storage performance that surpasses the upper bound of the Ragone plots of the current state‐of‐the‐art SCs. In addition, all‐solid‐state SCs with outstanding bending/folding durability are successfully demonstrated. Overall, these results provide critical insight into surface utilization of carbon electrodes as well as capacitive energy storage, when viscous and bulky ILs or ionogels are used as electrolytes.