and transition metal oxides (TMOs) [13][14][15][16] have recently been explored as promising anode candidates.TiO 2 , among other TMOs, is particularly attractive owing to its fascinating features including high structural stability, long cycle life, low cost, and high safety. [17][18][19][20][21] TiO 2 (B), as an unusual polymorph (bronze-phase) of TiO 2 , is found to have an open-channel structure and display a pseudo-capacitive behavior, thus enabling easier Li + diffusion and faster chargingdischarging capabilities. [ 22 ] Its theoretical capacity (335 mA h g −1 ) therefore significantly surpasses that (≈170 mA h g −1 ) of anatase or rutile TiO 2 , and is comparable to that (372 mA h g −1 ) of graphitic carbons. In consequence, various TiO 2 (B) nanostructures in the form of, e.g., nanoparticles, [23][24][25] nanorods, [ 26,27 ] nanowires, [28][29][30][31] nanotubes, [32][33][34][35][36] or nanosheets, [ 37,38 ] have been intensively studied as LIB anodes.It is worth noting, however, that the poor intrinsic conductivity of TiO 2 (B) inevitably sets obstacles for its applications as a high-power anode material. In this context, various carbonaceous materials, e.g., activated carbon fabrics, [ 39 ] carbon coatings, [ 40 ] carbon nanotubes, [ 41 ] or graphene nanosheets, [42][43][44][45] are introduced as conductive additives to ease the electron transport, thereby improving the cycle performances of TiO 2 (B) at high rates. Despite this progress, the reversible capacity of TiO 2 (B) is still insuffi cient, especially when compared to other TMOs, such as Fe 2 O 3 , [46][47][48][49][50] SnO 2 , [51][52][53][54] Co 3 O 4 , [ 55 ] and MnO 2 , [ 56 ] all of which boast of their much higher theoretical capacities (800−1200 mA h g −1 ) than TiO 2 (B).In this work, we expect to address the conductivity and capacity defi ciencies of TiO 2 (B) through a smart morphological and compositional design, aiming to achieve excellent reversible capacities and rate capabilities at the same time. Here we report elaborately designed hierarchical heterostructures, consisting of carbon-coated TiO 2 (B) nanosheets decorated with Fe 3 O 4 nanoparticles, based on a one-step self-assembly strategy through van der Waals interactions. [ 57 ] We stress that compared to other hybridization approaches based on hydrothermal synthesis, [46][47][48][50][51][52][53]55,56 ] atomic layer deposition, [ 49 ] and thermal pyrolysis, [ 54 ] our one-step self-assembly strategy is really facile and energy-effi cient, since it does not require harsh