While great progress has been achieved in the synthesis of ordered mesoporous carbons in the past decade, it still remains a challenge to prepare highly graphitic frameworks with ordered mesoporosity and high surface area. Reported herein is a simple synthetic methodology, based on the conversion of self-assembled superlattices of Fe 3 O 4 nanocrystals, to fabricate highly ordered mesoporous graphene frameworks (MGFs) with ultrathin pore walls consisting of three to six stacking graphene layers. The MGFs possess facecentered-cubic symmetry with interconnected mesoporosity, tunable pore width, and high surface area. Because of their unique architectures and superior structural durability, the MGFs exhibit excellent cycling stability and rate performance when used as anode materials for lithium-ion batteries, thus retaining a specific capacity of 520 mAh g À1 at a current density of 300 mA g À1 after 400 cycles.Nanostructured carbons, [1][2][3][4][5][6][7][8] including carbon nanotubes, [2] graphene, [3] and porous carbons, [4][5][6][7][8] represent an innovative class of technologically important materials. In particular, ordered mesoporous carbons (OMCs) with pore sizes tunable in the range of 2-50 nm have attracted increasingly greater attention because of their ordered mesoporosity, high surface area, and adjustable pore symmetry, [5] which have found wide applications in energy storage devices such as lithium-ion batteries (LIBs) and supercapacitors.[1a] Current methods of preparing OMCs rely on a templating strategy.[5] Both mesoporous silica and silica opals have been widely employed as hard templates to prepare OMCs through a nanocasting mechanism. [6, 7] More recently, block co-polymers have been used as a soft template for the direct synthesis of OMCs, [8] in analogy to the preparation of ordered mesoporous silica. [9] In spite of the aforementioned synthetic progress, most OMCs obtained to date are amorphous in nature, [6][7][8] and it may limit their applications, as the physicochemical properties (electronic conductivity and chemical stability, etc.) of porous carbon materials strongly depend on the crystallinity (i.e., graphitization degree) of the pore walls.[10] Highly graphitic porous carbons are attainable by heating the preformed OMCs at high temperatures (> 2500 8C), [11] which unfortunately can lead to the loss of surface area and structural ordering arising from pore collapse. Graphitic mesoporous carbons can also be realized at relatively low temperatures (< 1500 8C) by introducing metals or metal oxides as graphitization catalysts.[12] Despite the possibility to preserve the structural ordering by using this strategy, the resulting carbon frameworks are usually partially graphitic or semigraphitic as a result of the low graphitization temperature. Therefore, it still remains a challenge to synthesize highly graphitic frameworks with well-defined mesoporosity and high surface area.[13]Herein, we report a strategy of preparing highly ordered mesoporous graphene frameworks (MGFs) w...