Deciphering the determinants of starch digestion from multiple interrelated properties is a challenge that can benefit from multifactorial data analysis. The present study investigated the digestion kinetic parameters (rate, final extent) of size-fractions from four commercial wheat starches with different amylose contents. Each size -fraction was isolated and characterized comprehensively using a large range of analytic techniques (FACE, XRD, CP-MAS NMR, time-domain NMR, DSC...). A statistical clustering analysis applied on the results revealed that the mobility of water and starch protons measured by time-domain NMR was consistently related to the macromolecular composition of the glucan chains and to the ultrastructure of the granule. The final extent of starch digestion was determined by the granule structural features. The digestion rate coefficient dependencies, on the other hand, changed significantly with the range of granule size, i.e. the accessible surface for initial binding of alpha-amylase. The study particularly showed the molecular order and the chains mobility predominantly limiting or accelerating the digestion rate depending on the accessible surface. This result confirmed the need to differentiate between the surface and the inner-granule related mechanisms in starch digestion studies.