In this paper, we have reviewed the experimental and theoretical studies on pressure-induced polygonization, ovalization, racetrack-shape deformation, and polymerization of carbon nanotubes (CNTs). The corresponding electronic, optical, and mechanical changes accompanying these behaviors have been discussed. The transformations of armchair (n, n) CNT bundles (n = 2, 3, 4, 6, and 8) under hydrostatic or nonhydrostatic pressure into new carbons, including recently proposed superhard bct-C4, Cco-C8, and B-B1AL2R2 carbon phases have also been demonstrated. Given the diversity of CNTs from various chiralities, diameters, and arrangements, pressure-induced CNT polymerization provides a promising approach to produce numerous novel metastable carbons exhibiting unique electronic, optical, and mechanical characteristics.