Contrary to the observed positive giant magnetoresistance (GMR) in as-received multi-walled carbon nanotubes (MWNTs), pure polyaniline (PANI) synthesized with Cr(VI) as oxidant and MWNTs/PANI nanocomposites with ammonium persulfate (APS) as oxidant, a room temperature negative GMR of around ?2% was reported in MWNTs/PANI nanocomposites with Cr(VI) as oxidant. Different from a frequency switch of permittivity from negative to positive in MWNTs/PANI nanocomposites with APS as oxidant, unique negative permittivity was observed in MWNTs/PANI nanocomposites with Cr(VI) as oxidant within the measured frequency range from 20 to 2 × 106 Hz. The obtained unique negative permittivity was explained by the plasma frequency from the Drude model, at which the permittivity changes from negative to positive and the material changes from a metamaterial to an ordinary dielectric medium. The observed positive and negative GMR behaviors in these disordered systems as verified by the temperature dependent resistivity exploration were well explained through a wave-function shrinkage model and orbital magnetoconductivity theory by calculating the changed localization length (a0).