To reach the crucial milestone of generating efficient decarbonization pathways in sustainable concrete constructions, new technological developments to increase carbon sequestration in concrete are needed, well beyond the current carbon mitigation approaches limited to cement manufacturing. The objective of this presentation is to design sustainable and eco-friendly concrete by replacing cement with carbon-based agricultural byproducts and reinforcing it with graphene-based nanomaterials. This is a promising way for developing eco-efficient and highly resilient concrete, with at least 2x increased tensile load carrying and strain energy absorption capability; and 2-3x higher CO2 sequestration ability. The output of the proposed study will help promoting low-cost pathways for nullifying the greenhouse gas emission in the concrete and construction industry, while optimizing concrete’s carbon uptake and mineralization capacity, by engineering the nanostructured interfaces to accelerate carbonation kinetics.