To increase the viability of electric vehicles for the general population, it is critically important that rechargeable batteries are de-signed to support rapid charging, which is as important as increasing their energy density. However, commercial lithium-ion batteries (LIBs) encounter a ceiling of rate capability due to the sluggish intercalation kinetics of graphite anodes originated from their narrow interlayer spacing. Here, we report on graphite oxide frameworks (GOFs), whose interlayers are enlarged between 7.4 and 13 angstrom via a solvothermal reaction employing alpha, omega-diamino organic fillers. The GOFs offer ultrafast charging properties with a high lithium storage capacity of 370 mA h g(-1) (at 3,000 mA g(-1)). In addition, we could determine the optimum interlayer spacing of layered electrode materials, at which the barrier for Li+ transport could be minimized. Altogether, our findings provide deep insight for the rational design fast chargeable LIBs with electrodes based on layered materials.