www.advmat.degraphene-based 3D architectures with superhydrophobic and superoleophilic properties have demonstrated a remarkable performance for separation and absorption of oils or organic solvents from water. For instance, hydrophobic CNT sponges prepared from randomly (i.e., nonaligned) interconnected CNTs and exhibiting a contact angle of about 156° for water droplets were of great utility for environmental applications because of their capability to absorb and remove different types of oil from aqueous biphasic systems. [11,12] Meanwhile, graphene sponges have been more widely used for the absorption and separation of petroleum products, vegetable oils, and organic solvents from water. [13][14][15] In recent years, substitution of regular organic solvents by ionic liquids (ILs)molten salts with melting points below 100 °C-occurred in many diverse fields including catalysis, electrochemistry, separation and purification, or cellulose dissolution, among others., [16,17] For instance, in electrochemistry, the negligible vapor pressure of ILs makes them safer than regular organic electrolytes while preserving a wide operational electrochemical window-more so than that of aqueous ones. [18][19][20][21] However, hygroscopicity is quite common in ILs (even in hydrophobic ones) [22][23][24] becoming eventually a serious limitation for their practical use as electrolytes. [25] Moreover, ILs have also been used as catalysts or CO 2 sorbents, thus being regarded as "green solvents" because their negligible vapor pressure offered a more friendly alternative, in environmental terms, to common organic solvents used in industrial processes. Nonetheless, recent works have reported on contamination of aquatic environments with toxic and/or nonbiodegradable ILs. [26,27] Number of processes have been described for separation and purification of ILs, including adsorption, [28] extraction, [29] membrane separation, [30] crystallization, [31] distillation, [32,33] and supercritical-CO 2 -based extraction or precipitation, [34,35] i.e., with supercritical CO 2 playing the role of either a cosolvent or an antisolvent, respectively. Unfortunately, many of these processes are high cost and/or require high-energy input, and the purity of the recovered IL is yet an issue, mainly in terms of remaining water content. [36] Among them, adsorption is particularly interesting as it is a robust and nondestructive process for the recovery of ILs. In this regard, activated carbons Ionic liquids (ILs) are being widely used in many diverse areas of social interest, including catalysis, electrochemistry, etc. However, issues related to hygroscopicity of many ILs and the toxic and/or nonbiodegradable features of some of them limit their practical use. Developing materials capable of IL recovery from aqueous media and dehydration, thus allowing their recycling and subsequent reutilization, in a single and efficient process still poses a major challenge. Herein, electrically conductive aerogels composed of carbon nanofibers (CNFs) with remarkable sup...