In this chapter, we will discuss the potential of aluminum incorporation in C-S-H for enhancing its cryogenic stability. It systematically analyzes the atomistic structure of calcium-aluminosilicate-hydrate (C-A-S-H) with varying calcium and aluminum contents, revealing the stability of low-aluminum and high-aluminum C-A-S-H nanostructures under cryogenic attack. It turns out that the atomistic structure of low-aluminum C-A-S-H can remain stable, which enhances the stability in C-S-H pore structure and nanomechanical properties. Moreover, the presence form of aluminates in C-A-S-H is discussed here, further expanding the understanding of the existing C-A-S-H nanostructures. A DNA-code rule is introduced to describe and construct molecular models of C-A-S-H. We also propose a generalized structural-chemical formula for C-A-S-H models which can describe both cross-linked and non-cross-linked structures.