The functionalization of halloysite nanotubes (HNTs) has attracted much attention in recent years due to the nano-tubular structure and particular features. Here, we report a conductive nanohybrids of HNTs, polyaniline (PANI), and poly(sodium-p-styrenesulfonate) (PSS) with high electrical conductivity (0.11 S/cm) prepared by in situ polymerization and layer-by-layer assembly. The chemical structures and morphologies were characterized by FT-IR, UV-Vis, FE-SEM, and TEM, which confirmed that the layers of PANI, PSS, and PANI were sequentially coated onto the HNTs as expected. A study of cyclic voltammetry suggested the typical pseudocapacitance and good rate performance of the as-prepared nanocomposites. The results of galvanostatic charge/discharge and electrochemical impedance spectroscopy further demonstrated its favorable capacitive behavior and low resistance. The easily fabricated halloysite/polyaniline nanocomposites show great potential as electrode materials for supercapacitors.