The local dynamics of polypropylene (PP) in solution is studied by C-13 NMR relaxation and by molecular dynamics (MD) simulation via the orientational autocorrelation function (OACF) of C-H bonds. The interpretation protocol of this function proposed by Dejean de la Batie, Laupretre and Monnerie (DLM) [R. Dejean de la Batie, F. Laupretre, and L. Monnerie, Macromolecules 21, 2045(1988)] is applied and tested on new NMR measurements of the various microstructures of polypropylene. This interpretation scheme of the OACF is supported by a detailed study employing simulated PP trajectories in an atomistic heat bath. MD simulations indicate that, quite generally, the correlation time for segmental motions, tau(1), extracted from the DLM motional model is closely linked with the mean time between conformational jumps. Both experiments and simulations suggest a slightly higher mobility of meso sequences by comparison with racemic sequences. Our analysis of the microscopic aspects of the segmental dynamics and its manifestation in motional models allows us to trace the microscopic origin of the larger mobility of meso sequences.