The dynamically flexible lattices in lead halide perovskites may play important roles in extending carrier recombination lifetime in 3D perovskite solar-cell absorbers and in exciton self-trapping in 2D perovskite white-light phosphors. Two-dimensional infrared (2D IR) spectroscopy was applied to study a recently reported Pb-I-SCN layered perovskite. The Pb-I-SCN perovskite was spin-coated on a SiO2 surface as a thin film, with a thickness of similar to 100 nm, where the (SCN-)-C-12 anions were isotopically diluted with the ratio of (SCN)-C-12:(SCN)-C-13 = 5:95 to avoid vibrational coupling and excitation transfer between adjacent SCN- anions. The (CN)-C-12 stretch mode of the minor (SCN-)-C-12 component was the principal vibrational probe that reported on the structural evolution through 2D IR spectroscopy. Spectral diffusion was observed with a time constant of 4.1 +/- 0.3 ps. Spectral diffusion arises from small structural changes that result in sampling of frequencies within the distribution of frequencies comprising the inhomogeneously broadened infrared absorption band. These transitions among discrete local structures are distinct from oscillatory phonon motions of the lattice. To accurately evaluate the structural dynamics through measurement of spectral diffusion, the vibrational coupling between adjacent SCN- anions had to be carefully treated. Although the inorganic layers of typical 2D perovskites are structurally isolated from each other, the 2D IR data demonstrated that the layers of the Pb-I-SCN perovskite are vibrationally coupled. When both (SCN-)-C-12 and (SCN-)-C-13 were pumped simultaneously, cross-peaks between (SCN)-C-12 and (SCN)-C-13 vibrations and an oscillating 2D band shape of the (SCN-)-C-12 vibration were observed. Both observables demonstrate vibrational coupling between the closest SCN- anions, which reside in different inorganic layers. The thin films and the isotopic dilution produced exceedingly small vibrational echo signal fields; measurements were made possible using the near-Brewster's angle reflection pump-probe geometry.