Carbon nanotube (CNT) is a type of carbon allotrope with excellent physical and electrical properties, including high thermal conductivity, mechanical strength, and thermal stability. Therefore, applications of CNT have been considered for a variety of fields, including biosensors, molecular electronics, X-ray, and fuel cells. However, the application of CNT to biomedicine is limited because this material is cytotoxic and inhomogeneous. In particular, the irregularity in the structural properties of paste or bundle-type CNTs causes an uncontrolled modification in biomolecules. Therefore, using CNT as biosensors to obtain quantitative analyses is difficult. In this study, we developed a new method to perform end-selective functionalization of CNT in order to enable quantitative analysis for biomedical applications. The process was as follows: (1) etching the tip of vertically-aligned CNTs under optimum conditions, (2) oxidation of exposed CNTs, and (3) end-selective linkage of functionalized CNTs with biomolecules (dsDNA).