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A novel high-performance multiwalled carbon nanotube (MWCNT) nanocomposite (MWCNT?TLCP) was prepared using an in situ polycondensation approach by grafting a thermotropic liquid-crystalline polymer (TLCP) onto the sidewalls of MWCNTs functionalized with hydroxyphenyl groups. FTIR spectroscopy revealed that TLCP was covalently attached to the MWCNTs, and Raman signals corresponding to the D- and G-bands of MWCNTs were attenuated after functionalization. TEM and TGA results showed that the average thicknesses of grafted TLCP layers on the MWCNT surface were 5?7 nm, and the amount of grafted TLCP was about 56 wt %. The morphology of MWCNT?TLCP/TLCP composite containing 3 wt % liquid-crystalline polymer-modified MWCNTs was examined by SEM. SEM images of the composite fracture surfaces showed a homogeneous dispersion of the MWCNT?TLCP nanocomposite in the TLCP matrix. The mesophase temperature region of the composite was obviously increased because of the presence of functionalized MWCNTs.