The hydrogen sorption behavior of novel Pd-doped sepiolite-derived carbon nanofibers (SDCNs) was investigated. Two chemical doping methods of ethanol/ toluene reduction and a polyol process were applied to control Pd(0) formation in the SDCNs at different Pd doping levels. Hydrogen storage capacity was observed to vary depending on the Pd particle size and doping amount as the Pd particle surface area and the carbon Brunauer-Emmett-Teller (BET) surface area change with them, suggesting the existence of an optimum Pd doping level at each doping method for the best hydrogen storage capacity. Among the samples prepared using the polyol method at different Pd amounts, the maximum hydrogen uptake of about 0.41 wt % was obtained at 298 K and 90 bar for the 5 wt % Pd-doped SDCN that has a relatively high Pd particle surface area and carbon BET surface area. Samples prepared using the ethanol/ toluene reduction method exhibited a higher hydrogen uptake of about 0.59 wt % at lower Pd doping levels (3 wt % Pd) due to a smaller Pd particle size and relatively high carbon BET surface area. The hydrogen desorption behavior investigated by differential scanning calorimeter exhibited that a higher amount of hydrogen desorbed at around 860 K from the Pd-doped SDCNs compared to that from the undoped SDCN. Fourier transform infrared (FTIR) spectroscopic analysis suggested that some of the weak chemisorbed hydrogen changes to a normal covalent bond during the heating and effuses at around 860 K.