LIBs are being promoting to power electric vehicles. [3] To address these issues, various approaches have been developed. One approach is to use flame retardant additives in electrolytes, such as fluorinated alkyl phosphates and hexamethylphosphoramide. [4] Inorganic solid-state electrolytes have also been investigated to replace organic liquid electrolytes because they are nonflammable and have high enough mechanical strength to prevent dendritic lithium from penetrating the electrolyte. [5] However, the relatively low ionic conductivity at room temperature and large interfacial resistance has limited the large-scale applications of all solidstate lithium batteries. [6] On the other hand, aqueous electrolyte could be the ideal solution to overcome safety issues due to its nonflammable nature and because the excellent kinetics of electrode materials in liquid environments can significantly outperform the solid state counterparts. [7] Aqueous electrolytes have had a long history of development. Among various aqueous batteries, lead-acid batteries using sulfuric acid as electrolyte were invented in 1859 and are still widely used in automobiles for starting, ignition, and lighting. For other aqueous battery systems, Xia and co-workers developed aqueous electrolytes in LIB system, where they found the side reactions between electrodes and water/oxygen resulted in rapid loss of capacity. An excellent cycling stability can be achieved by eliminating oxygen from electrolyte and modifying electrodes. [7c] To further exploit the advantages of highcapacity lithium metal anodes in aqueous electrolyte systems, lithium metal was coated by a bilayer lithium ion conductor and the full cell exhibited a much higher output voltage and improved energy density. [8] Most recently, Suo et al. proposed a new "water-in-salt" concept to increase the concentration of aqueous electrolyte, which can effectively broaden the potential window of aqueous electrolyte and enable a new battery system with both high energy density and promising safety. [9] Battery systems using aqueous electrolytes have presented great progress, however there has been little investigation on current collectors for aqueous battery systems. Presently, typical current collectors used in aqueous battery systems are metal-based materials, which are heavy, expensive, bulky and Lithium-ion batteries (LIBs) are integral parts of modern technology, but can raise safety concerns because of their flammable organic electrolytes with low flash points. Aqueous electrolytes can be used in LIBs to overcome the safety issues that come with organic electrolytes while avoiding poor kinetics associated with solid state electrolytes. Despite advances in aqueous electrolytes, current collectors for aqueous battery systems have been neglected. Current collectors used in today's aqueous battery systems are usually metal-based materials, which are heavy, expensive, bulky, and prone to corrosion after prolonged use. Here, a carbon nanotube (CNT)-cellulose nanofiber (CNF) all-fiber com...