The evolution of concrete materials faces challenges in meeting the mechanical demands of contemporary architectural structures due to the limitations of conventional concrete and the impracticalities of ultra-high-performance concrete. Addressing this, the exploration of Low-Carbon, High-Performance Cement-Based Composites (LCHPCC) emerges as a strategic avenue. This paper investigates diverse materials within the LCHPCC realm, emphasizing material selection and innovative processes to bolster performance and sustainability. The study delves into large-volume pozzolanic cementitious materials, including the limestone-calcined clay-cement (LC³) system, inert filler powders, and alkali-activated systems. It underscores critical considerations for optimizing powder material utilization in low-carbon methodologies. Furthermore, enhancing the aggregate system with low-carbon fine and coarse aggregates enhances the high-performance and low-carbon characteristics of LCHPCC. Incorporating recycled waste fibers significantly increases the mechanical properties of LCHPCC. Additionally, the integration of specific chemical additives and nanomaterials not only elevates performance but also broadens the application potential of LCHPCC. A life-cycle assessment analysis and practical validation case studies demonstrate the substantial advantages of LCHPCC over traditional concrete, emphasizing its sustainable attributes. This paper offers a balanced proposition for the ongoing development of low-carbon concrete materials, aligning with the principles of sustainable construction.