The production of concrete leads to substantial carbon emissions (~8%) and includes reinforcing steel which is prone to corrosion and durability issues. Carbon-fiber-reinforced concrete is attractive for structural applications due to its light weight, high modulus, high strength, low density, and resistance to environmental degradation. Recycled/repurposed carbon fiber (rCF) is a promising alternative to traditional steel-fiber reinforcement for manufacturing lightweight and high-strength concrete. Additionally, rCF offers a sustainable, economical, and less energy-intensive solution for infrastructure applications. In this paper, structure-process-property relationships between the rheology of mix design, carbon fiber reinforcement type, thermal conductivity, and microstructural properties are investigated targeting strength and lighter weight using three types of concretes, namely, high-strength concrete, structural lightweight concrete, and ultra-lightweight concrete. The concrete mix designs were evaluated non-destructively using high-resolution X-ray computed tomography to investigate the microstructure of the voids and spatially correlate the porosity with the thermal conductivity properties and mechanical performance. Reinforced concrete structures with steel often suffer from durability issues due to corrosion. This paper presents advancements towards realizing concrete structures without steel reinforcement by providing required compression, adequate tension, flexural, and shear properties from recycled/repurposed carbon fibers and substantially reducing the carbon footprint for thermal and/or structural applications.