Halloysite nanotubes/polypyrrole (HNTs/PPy) nanocomposites with coaxial tubular morphology for use as electrode materials for supercapacitors were synthesized by the in situ chemical oxidative polymerization method based on self-assembled monolayer amine-functionalized HNTs. The HNTs/PPy coaxial tubular nanocomposites were characterized with transmission electron microscope (TEM), X-ray diffraction (XRD), thermogravimetric analysis (TGA), electrical conductivity measurement at different temperatures, cyclic voltammetry (CV), and galvanostatic charge–discharge measurements. The coaxial tubular nanocomposites showed their greatest conductivity at room temperature and a weak temperature dependence of the conductivity from 298K to 423K. A maximum discharge capacity of 522F/g after correcting for the weight percent of the PPy phase at a current density of 5mAcm−2 in a 0.5M Na2SO4 electrolyte could be achieved in a half-cell setup configuration for the HNTs/PPy composites electrode, suggesting its potential application in electrode materials for electrochemical capacitors.