In this work, we developed a convenient and efficient method for solubilization, purification and functionalization of carbon nanotubes (CNTs) using a versatile reagent (phosphotungstic acid (HPW)). Because HPW can spontaneously attach to graphite walls as polyanions and provide static repulsion, CNT aggregates were divided into individual and small bundles of CNTs and turned into a stable solution by sonication in the presence of HPW. Amorphous carbon impurities and metal catalysts in the raw CNTs were removed by centrifugation and filtration. Finally, purified CNTs with a yield of 82 wt% were obtained. Using HPW on graphite walls as an electrostatic and acid anchor, positively charged titania nanoparticles and albumin molecules were successfully assembled around CNTs without altering their delocalized π-electron system. The versatility of this simple approach could be extended beyond inorganic nanoparticles and proteins, to other systems with desired properties.