The doping of SiO2 and Fe2O3 into hydrochars that were produced by the hydrothermal carbonization of cellulose was studied with respect to its impact on the resulting surface characteristics and sorption behavior of CO2, CH4, and O2. During pyrolysis, the structural order of the Fe-doped char changed, as the fraction of highly ordered domains increased, which was not observed for the undoped and Si-doped chars. The Si doping had no apparent influence on the oxidation temperature of the hydrochar in contrast to the Fe-doped char where the oxidation temperature was reduced because of the catalytic effect of Fe. Both dopants reduced the micro-, meso- and macroporous surface areas of the chars, although the Fe-doped chars had larger meso- and macroporosity than the Si-doped char. However, the increased degree in the structural order of the carbon matrix of the Fe-doped char reduced its microporosity relative to the Si-doped char. The adsorption of CO2 and CH4 on the chars at temperatures between 273.15 and 423.15 K and at pressures up to 115 kPa was slightly inhibited by the Si doping but strongly suppressed by the Fe doping. For O2, however, the Si doping promoted the observed adsorption capacity, while Fe doping also showed an inhibiting effect.