Concrete is the most widely used construction material in the world and is responsible for 7% of global carbon emissions. It is inherently brittle, and it requires frequent repair or replacement which is economically expensive and further generates large volumes of carbon dioxide. Current methods of repair by agents such as mortar, epoxies, and bacteria result in structures with reduced strength and resiliency. Recent advances in the design of structural composites often mimic natural microstructures. Specifically, the structure of abalone nacre with its high stiffness, tensile strength, and toughness is a source of inspiration from the process of evolution. The inspiration from nacre can lead to design of a new class of architected structural materials with superb mechanical properties. This body of work first presents a method to reinforce concrete with an architected polymer phase. Second is presented how a ubiquitous enzyme, Carbonic anhydrase (CA), can be used to repair and strengthen cracked concrete, and how it can be used as an additive in fresh concrete. The first study presents an experimental and computational study on a set of bioinspired architected composites created using a cement mortar cast with brick-and-mortar and auxetic polymer phases. The impact of this unit-cell architected polymer phase on the flexural and compressive strengths, resilience, and toughness is studied as a function of microstructural geometry. All mechanical properties of the architected composite samples are found to be greater than those of control samples due to prevention of localized deformation and failure, resulting in higher strength. The microstructurally designed composites showed more layer shear sliding during fracture, whereas the control samples showed more diagonal shear failure. After initial cracking, the microstructurally designed composites gradually deformed plastically due to interlocking elements and achieved high stresses and strains before failure. Results also show that microstructurally designed composites with the architected polymer phase outperform control samples with equal volume fraction of a randomly oriented polymer fiber phase. Computational studies of the proposed unit cells are also performed, and the results suggest that the orientation of cells during loading is critical to achieve maximum performance of a cementitious composite. The implications of these results are immense for future development of high performing construction materials. The second study outlines methods for repair of concrete and lays the groundwork to develop a self-healing concrete that uses trace amounts of the CA enzyme. The CA catalyzes the reaction between calcium ions and carbon dioxide to create calcium carbonate that naturally incorporates into concrete structures with similar thermomechanical properties as concrete. The reaction is safe, actively consumes carbon dioxide, generates low amounts of heat, and avoids using unhealthy reagents, resulting in a strong structure. This repair method results in concrete samples with similar strength and water permeability as the intact materials. These results offer an inexpensive, safe, and efficient method to create self-healing concrete structures. The science underlying the creation of self-healing concrete is described, producing a material intrinsically identical to the original using the CA enzyme. Using this strategy, a preliminary self-healing concrete mix is able to self-repair fractures via hydration. This body of work addresses a major issue: Is there an efficient and ecological repair for decaying concrete infrastructure? These methods propose alternative reinforcement, alleviates high monetary and energy costs associated with concrete replacement, and consume the greenhouse gas, carbon dioxide.