A covalent route has been successfully utilized for the surface modification of ordered mesoporous carbon (OMC) CMK-3 by in situ polymerization and grafting of methyl methacrylate (MMA) in the absence of any solvent. The modified CMK-3 carbon particles have a high loading of 19 wt% poly(methyl methacrylate) (PMMA), named PMMA-g-CMK-3, and also maintain their high surface area and mesoporous structure. The in situ polymerization technique endows a significantly enhanced electric conductivity (0.437 S m(-1)) of the resulting PMMA-g-CMK-3/PMMA composite, about two orders of magnitude higher than 1.34 × 10(-3) S m(-1) of PMMA/CMK-3 obtained by the solvent mixing method. A minimum reflection loss (RL) value of -27 dB and a broader absorption band (over 3 GHz) with RL values <-10 dB are obtained for the in situ polymerized PMMA-g-CMK-3/PMMA in a frequency range of 8.2-12.4 GHz (X-band), implying its great potential as a microwave absorbing material. The maximum absorbance efficiency for the in situ polymerized sample increases remarkably compared to that (-10 dB) of CMK-3/PMMA prepared by the solvent mixing method. Changing the thickness of the absorber can efficiently adjust the frequency corresponding to the best microwave absorbance ability. The enhanced microwave absorption by the surface modified CMK-3 is ascribed to high dielectric loss. This in situ polymerization for the surface modification of mesoporous carbons opens up a new method and idea for developing light-weight and high-performance microwave absorbing materials.