Carbon nanotube/poly(vinylidene fluoride) (CNT/PVDF) composites were prepared using CNT with different oxidation and thermal treatments. The oxidation procedure leads to CNT with the most acidic characteristics that lower the degree of crystallinity of the polymer and contribute to a large increase of the dielectric constant. The surface treatments, in general, increase the percolation threshold and decrease conductivity. The surface treatments do not seem to affect CNT interactions and similar degrees of dispersion are achieved in all cases, as shown by the SEM results. The maximum value of the dielectric constant is similar to 630. It is demonstrated that the composite conductivity can be attributed to a hopping mechanism that is strongly affected by the surface treatment of the CNT.