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In this study, hexagonal boron nitride nanosheets grafted with aliphatic groups (Alkyl-BN) were synthesized by a sonication-assisted alcoholysis reaction using hexagonal boron nitride (hBN) with 1-dodecanol, and a series of polypropylene (PP) nanocomposites were prepared by mixing PP with different amount of Alkyl-BN. The PP/Alkyl-BN nanocomposite containing a very small amount of Alkyl-BN showed much improved mechanical properties than those of neat PP and PP/hBN nanocomposites. For instance, Young's modulus value of PP/Alkyl-BN nanocomposite containing 0.5 wt% of Alkyl-BN is larger than that of neat PP by 17.5% while that of PP/hBN nanocomposite containing 0.5 wt% of hBN is larger by only 1.2%. The tensile strength value of PP/Alkyl-BN was found to be larger than that of the neat PP by 7.4% due to the enhanced interfacial interaction between Alkyl-BN and PP chains. Furthermore, the PP/Alkyl-BN nanocomposites exhibited enhanced thermal conductivity and stability than the neat PP and PP/hBN nanocomposite. This research clearly shows that the improved thermal and mechanical properties of polymer nanocomposites can be achieved with a very low filler content by the enhancement of the interfacial interaction between the filler materials and the polymer matrix.