The structural basis of the interdependence between moisture content and mechanical properties in natural cellulose is explored using a solid state NMR experiment which is sensitive to cellulose chains on the surface of unitary crystallite. Making assumptions based on current knowledge of biosynthesis of cellulose, and the dipolar transport of magnetisation in solids, it is shown that the sorption of moisture causes the activation of cooperative motion of cellulose chains on the surface of the cellulose crystallite in a manner which is related to the moisture content. An important implication for these results is that densification of cellulose and associated changes in the water sorption isotherm, is structural relaxation on the nano, or unitary crystallite scale. The results is also discussed in term of the evolving and modern picture of cellulose.