An ordered structure and high mechanical property of calcium silicate hydrate (C-S-H) gel has been always pursued in the field of cementitious materials. In this paper, compacted and layer-by-layer stacking C-S-H plates were fabricated based on Layer-by-Layer (LBL) method and H-cell penetration (HCP) method through cation exchange membrane templating. This new way changed the randomly packing structure of traditional C-S-H, and synthesized a high-orderly C-S-H platelets with denser structure. Based on molecular dynamics simulations, it can be attributed to the strong adsorption and nucleation sites contributed by sulfonic acid groups on the cation exchange membrane. Besides, AFM indentation experiments indicate this C-S-H owns significantly higher elastic modulus than traditional C-S-H, while the mechanical properties can be further increased by the addition of PVA and the regulation of reaction time. This new type C-S-H may pave the way to the preparation of high-performance concrete in the future.