Much of the existing knowledge on the nanostructure of cementitious Calcium Silicate Hydrate (C-S-H) nanoparticles has been gained from structural comparisons with crystalline calcium silicate hydrates. In fact, several models [1-5] have been proposed so far that draw structural analogies with tobermorite and jennite crystals and/or with distorted semi-crystalline variations of them (the so called C-S-H (I) and C-S-H (II) phases respectively). From these models, CS-H gels can be approximately viewed as layered structures, in which calcium oxide sheets are ribbed on either side with silicate chains, and free calcium ions and water molecules are present in the interlayer space (see Figure). 1.4nm-Tobermorite Jennite