We presented a scalable fabrication method for the preparation of multilayered nano-prism vertex (NV)-tips whose dimensions can be controlled for tip-enhanced Raman spectroscopy (TERS). The NV-tip had sharp vertices (diameter ∼20 nm) originated from the chemical lift-off process after the angle-grinding process, enabling high resolution imaging. TERS measurements were performed on brilliant cresyl blue (BCB) molecules using a Ag/Au NV-tip, revealing the enhanced field localization at the vertices of the NV-tip. Furthermore, we could observe the polarization effect of the NV-tip. Our NV-tips should be a powerful tool for basic research on TERS experiments and SPM applications.