The electrical and rheological percolation behaviors of polycarbonate/multiwall carbon nanotube nanocomposites were investigated. To determine the effects of surface functionalization on a carbon nanotube surface, poly(styrene-co-acrylonitrile) (SAN)-grafted multiwall carbon nanotubes were prepared using surface-initiated atom transfer radical polymerization. The amount of grafted SAN was controlled by changing the polymerization time and was characterized using TGA. FT-IR and TEM were used to characterize the surface of the functionalized carbon nanotubes. The rheological and electrical percolation behaviors of the SAN-grafted multiwall carbon nanotube/polycarbonate nanocomposites were compared to those of pristine multiwall carbon nanotubes, where the effects were shown to increase with increasing SAN content. The results are attributed to the compatibility of SAN with polycarbonates, which induced uniform dispersion of the functionalized carbon nanotubes. Uniform dispersion was also confirmed by evaluating a tensile-fractured nanocomposite specimen.