A Carbon NanoTube (CNT) structure includes a substrate, a CNT support layer, and a plurality of CNTs. The CNT support layer is stacked on the substrate and has pores therein. One end of each of the CNTs is attached to portions of the substrate exposed through the pores and each of the CNTs has its lateral sides supported by the CNT support layer. A method of vertically aligning CNTs includes: forming a first conductive substrate; stacking a CNT support layer having pores on the first conductive substrate; and attaching one end of the each of the CNTs to portions of the first conductive substrate exposed through the pores.