With the rapidly increasing interests on wearable electronics over the past decades, the limited energy density and nondeformable configuration of conventional 2D lithium-ion batteries (LIBs) have already become the dominant obstacles that are hindering the roads of wearable consumer electronics toward ubiquity. [1][2][3][4][5] Hence, it is urgent to develop an alternative highperformance flexible energy storage device to break through the inherent restrictions of rigid LIBs. [6][7][8] The Li-CO 2 battery, a newly conceptual metal-gas battery, has been considered as a promising candidate for the next-generation high-performance electrochemical energy storage system recently. [9,10] It possesses a high theoretical energy density via the four-electrons transfer reaction (4Li + + 3CO 2 + 4e − → 2Li 2 CO 3 + C, E° = 2.80 V vs Li + /Li) and provides a novel environmentally friendly approach to CO 2 fixing which is of great benefit to alleviate global warming. [11][12][13] Interestingly, the Li-CO 2 battery is also very attractive for aerospace exploration; for example, it may be a possible energy system for providing electricity on Mars where the atmosphere consists of 96% CO 2 gas. [14] In spite of the aforementioned favorable factors, very few reports in the literature related to flexible Li-CO 2 battery devices for wearable electronics have been reported so far. After systematical investigations, it is found that the main challenges of fabricating high-performance flexible Li-CO 2 battery devices lie in the following three aspects: (1) carbon nanophases (e.g., Ketjenblack, [9,10,15] CNTs, [11,16] graphene [17,18] ), which dominate those known Li-CO 2 battery catalysts, induce the formation of Li 2 CO 3 , a wide-bandgap insulator. [19,20] It results in a sluggish kinetics for CO 2 evolution so that a high charge potential of 4.2-4.6 V was commonly required to drive the degradation of Li 2 CO 3 in most previous Li-CO 2 batteries. [10,11,17] Such high potential not only increases the risk of electrolyte decomposition but also accelerates the oxidation of electrodes. [21,22] Meanwhile, originated from the incomplete decomposition, more and more solid carbonate species accumulated in the surface of cathode during cycling, leading to a distinct decrease on catalytic performance and even the rapid extension of impedance up to a "sudden death" of the battery. [20,23,24] Consequently, the majority of those reported Li-CO 2 batteries showed a negligibleThe rapid development of wearable electronics requires a revolution of power accessories regarding flexibility and energy density. The Li-CO 2 battery was recently proposed as a novel and promising candidate for nextgeneration energy-storage systems. However, the current Li-CO 2 batteries usually suffer from the difficulties of poor stability, low energy efficiency, and leakage of liquid electrolyte, and few flexible Li-CO 2 batteries for wearable electronics have been reported so far. Herein, a quasi-solidstate flexible fiber-shaped Li-CO 2 battery with low overpotential and ...