Two-dimensional conjugated metal-organic frameworks (2D c-MOFs) have recently emerged for potential applications in (opto-)electronics, chemiresistive sensing, and energy storage and conversion, due to their excellent electrical conductivity, abundant active sites, and intrinsic porous structures. However, developing ultrathin 2D c-MOF nanosheets (NSs) for facile solution processing and integration into devices remains a great challenge, mostly due to unscalable synthesis, low yield, limited lateral size and low crystallinity.Here, we report a surfactant-assisted solution synthesis toward ultrathin 2D c-MOF NSs, including HHB-
Cu(HHB ¼ hexahydroxybenzene), HHB-Ni and HHTP-Cu (HHTP ¼ 2,3,6,7,10,11hexahydroxytriphenylene). For the first time, we achieve single-crystalline HHB-Cu(Ni) NSs featured with a thickness of 4-5 nm ($8-10 layers) and a lateral size of 0.25-0.65 mm 2 , as well as single-crystalline HHTP-Cu NSs with a thickness of $5.1 AE 2.6 nm ($10 layers) and a lateral size of 0.002-0.02 mm 2 . Benefiting from the ultrathin feature, the synthetic NSs allow fast ion diffusion and high utilization of active sites. As a proof of concept, when serving as a cathode material for Li-ion storage, HHB-Cu NSs deliver a remarkable rate capability (charge within 3 min) and long-term cycling stability (90% capacity retention after 1000 cycles), superior to the corresponding bulk materials and other reported MOF cathodes.