Carbon materials have received great attention owing to their numerous allotropes and rich properties. Structure design and property tuning of carbon materials is one of the tremendous challenges in the field of materials science research. Here we carried out a bottom-up approach and identified a series of carbon allotropes with similar structures but distinct properties. The structures designed in this work had comparable energy stability to those previously predicted using the top-down global structure search method. Theoretical property calculations demonstrated that the three carbon structures with pure sp3 hybridization possessed semiconductive and superhard properties, while the carbon structure with sp2 + sp3 hybridization exhibited metallic features. Also, they differed significantly in the anisotropy of the mechanical properties. These carbon structures had some match to the unidentified phases in the detonation soot and could hopefully be synthesized by thermal "degassing" of high-pressure Na-C products. Our results propose a strategy to regulate properties through structural tuning, thus paving a way for the design and synthesis of materials with desirable properties.