Reactive force field molecular dynamics was utilized to investigate the structure, dynamics, and mechanical nature of different cations solvated in the nanometer-channel of highly disordered calcium silicate hydrate. The local structures of different cations bonded with hydroxyl groups are characterized by the long spatial correlation, bond angel distribution preference, and featured coordinated number, resembling those of the tetra-/penta-/octahedron for cation-oxygen structure in the defective region of the silicate glass. Al atoms in the interlayer region play a role in bridging the defective silicate chains and enhance the connectivity of the silicate skeleton. Dynamically, the mobility of ultraconfined water molecules and cations is significantly influenced by the ionic chemistry: the residence time for water molecules in the hydration shell of Al and Mg ions is longer than that in the environment of Na and Ca ions. Furthermore, uniamial tension simulation provides insight that while both the stiffness and cohesive strength of the C-S-H gels are significantly improved due to the silicate-aluminate branch structure formation, sodium ions with unstable Na-O connection weaken the loading resistance of the C-S-H gels. During the tensile process, the hydrolytic reaction is also affected by the cationic type: water molecules coordinated with Al and Mg cations at high stress state are likely to decompose, but those aggregated with sodium ions are hard to be stretched broken due to the low failure stress.