Optimising the mesoscale structure of calcium-silicate-hydrate (C-S-H) is critical to achieving durable and sustainable infrastructure using Portland cement concrete. However, control of its intricate formation process, which comprises spatially disordered growth of poorly-crystalline sheets, remains a challenge. Here, through combination of experimental and computer simulation techniques, we report a promising mechanism to control this complex growth process and thereby optimise the C-S-H nanostructure. The pivotal step was utilizing graphene oxide (GO) to restrain the inherent spatial deformations of the C-S-H sheets and guide their concurrent 2D growth and layer-by-layer ordering. Accordingly, we designed a layered GO–C-S-H composite that exhibits 1–2 orders of magnitude improvement in strength and durability compared with C-S-H formed without control. Our findings open a window for nano-engineering of cements and other complex layered materials for ceramic, pharmaceutical and energy applications.

优化硅酸钙水合物 (CSH) 的中尺度结构对于使用波特兰水泥混凝土实现耐用和可持续的基础设施至关重要。然而，控制其复杂的形成过程，包括低结晶片的空间无序生长，仍然是一个挑战。在这里，通过实验和计算机模拟技术的结合，我们报告了一种有希望的机制来控制这种复杂的生长过程，从而优化 CSH 纳米结构。关键步骤是利用氧化石墨烯 (GO) 来抑制 CSH 片的固有空间变形，并引导它们同时进行 2D 生长和逐层排序。因此，我们设计了一种分层的 GO-CSH 复合材料，与未经控制形成的 CSH 相比，其强度和耐久性提高了 1-2 个数量级。我们的发现为水泥和其他用于陶瓷、制药和能源应用的复杂层状材料的纳米工程打开了一扇窗。