Solid-state NMR (ssNMR) is a unique technique allowing the study of macromolecular assemblies in their native state without prior modification. The proposed method simplifies the current long and tedious data-acquisition and processing protocols for Variable Contact Time (VCT) ssNMR experiments used in dynamic studies of macromolecular assemblies. Using cellulose nanocrystals as a model for polysaccharide assembly, the acquisition time was reduced by decreasing the number of scans and shortening the recycling time required for the H-1 to C-13 polarization transfers.A tenfold reduction in the acquisition time for each kinetic point was achieved while maintaining a good signal to noise ratio.The processing time for the pseudo-2D solid-state NMR data was also shortened by using signal intensities derived from peak picking rather than the classically-used spectral deconvolution method.These optimizations enabled the molecular dynamic parameters T-1 rho(H), T-HH, T-CH to be accessed within a day. (c) 2022 The Author(s). Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/)