Scientific organizations are creating carbon nanotube-based composites like V C 5 C 7 [ m , n ] and H C 5 C 7 [ m , n ] , which indicate significant response against voltage. Imbalance-based irregularity indices determine the degree of irregularity of a certain molecular structure and, as a result, determine the properties of a molecular substance. In this article, we aim to compute irregularity indices of two nanotubes, V C 5 C 7 [ m , n ] and H C 5 C 7 [ m , n ] . We produce formulas for the irregularity of these two nanotubes, which are functions depending on the parameters of the structure m and n . We compare our results graphically and conclude that V C 5 C 7 [ m , n ] is more irregular than H C 5 C 7 [ m , n ] .