Porphyrin tapes have attracted extensive attention because their fully conjugated π-networks act as nonlinear optical (NLO) materials. A family of Ni(II) and Zn(II) porphyrin arch-tapes that are connected by varying bridge (B) ligands (meso-meso β-β doubly linked dimer 1, meso-meso β-β β-β triply linked dimer 3, methylene-inserted dimer 2 and trimer 5, carbonyl-inserted dimer 4, trimer 6, and Zn(II) trimer 7) have been synthesized by a density functional theory (DFT) method. The results show that carbonyl-inserted arch-tapes significantly enhance second hyperpolarizability (γ), indicating that the remarkably contorted structure incorporated seven-membered ring(s) directly affect their NLO properties of our focus. Moreover, the electronic absorption spectra calculated for all studied complexes with time-dependent DFT theory (TDDFT) predict that carbonyl-inserted complex 4 contributes to a red-shift of the Q-band (160 nm) for the meso-meso β-β doubly linked complex 1. The third-order NLO responses and the electron transition properties strongly depend on the nature of the bridge (B) ligand, which means that an active involvement of the carbonyl group presents an advantage for its application in NLO materials.