Great efforts have been made toward the syntheses of nanocomposites of inorganic materials and carbon nanotubes (CNTs), [1][2][3][4][5] with the aim of exploiting the unique properties of CNTs (such as a high aspect ratio, low mass, flexibility, a high mechanical strength, and high electrical and thermal conductivities) for applications in heterogeneous catalysis, [2] fuel cells, [3] supercapacitors, [4] lithium-ion batteries (LIBs), [5] and optoelectronic devices.[6] The performances of these nanocomposites should be significantly affected by at least one of three key structural factors: uniformity, maintenance of the electrical contacts between CNTs, and porosity. Therefore, it is of fundamental interest to develop synthetic strategies for uniformly loading inorganic materials onto the surfaces of CNTs and CNT bundles within mesoporous sheets without disturbing the electrical contacts between the CNTs, so that such materials can be used in fuel cells, supercapacitors, and LIBs. To the best of our knowledge, the only previous attempt (in which layers of V 2 O 5 ÁxH 2 O with a 6 nm thickness were electrochemically loaded onto CNT films) had not been fully successful; aggregates were clearly observed on the surface of the films.[4b]Here, we report the uniform loading of SnO 2 nanoparticles (NPs) onto a CNT network composed of 1 Â 1 cross-stacked sheets (see Scheme S1, Supporting Information); the NPs are observed on the surface of each multiwalled CNT and of each CNT bundle within the network. This technique may be useful in the fabrication of high-capacity anodes for rechargeable LIBs. Additional considerations for the design of the novel composite arise because all three key factors are very important to this application.Tin-based materials have also attracted great attention as potential substitutes for current carbonaceous materials because of their higher specific capacities (981 mA h g À1 for Sn, 1491 mA h g À1 for SnO 2 , assuming that all Sn was oxidized to Sn 4þ , approximately 360 mA h g À1 for C-based materials). [7][8][9] However, anodes of such high capacity usually suffer severe capacity fading stemming from both the quick aggregation of tin particles and the huge volume change (over 300%) during Li þ insertion/extraction cycles, which causes pulverization of the anodes and electrical detachment of active materials. [9] Reducing the materials' size down to the nanoscale and dispersing the materials into mesoporous structures have proved very effective in solving the problems of similar systems.[5b,10] There have already been some reports of applying inorganic-CNT composites to high-capacity anodes for LIBs, [5b-d] but all of these composites were prepared using CNTs as collectors for sediments, so carbon black and polymer binders had to be used to lower the resistance and hold the electrodes together. In contrast, CNT sheets have been demonstrated to be very attractive candidates for freestanding (no need for copper foil substrates as current collectors) and binder-free anodes (no need for po...