Water dispersible nanofibrilar polyaniline (NF-PANI) provides a novel and direct route towards carbon nanotube water dispersions of high concentration. Carrying out the chemical synthesis of NF-PANI in the presence of carbon nanotubes (CNTs) results in an entirely nanostructured nanofibrilar polyaniline/carbon nanotube (NF-PANI/CNT) composite material that contains well segregated CNTs partially coated by NF-PANI. This new approach is simple, fast, and inexpensive, and enables the direct preparation of stable and homogeneous dispersions of the composites in water at concentrations up to 10 mg - mL(-1), even for the highest CNT loadings of 50 wt.-% without the participation of surfactants or stabilizers.