Preparing a lightweight yet high-strength bio-based structural material with sustainability and recyclability is highly desirable in advanced applications for architecture, new energy vehicles and spacecraft. In this study, we combined cellulose scaffold and aramid nanofiber (ANF) into a high-performance bulk material. Densification of cellulose microfibers containing ANF and hydrogen bonding between cellulose microfibers and ANF played a crucial role in enhanced physical and mechanical properties of the hybrid material. The prepared material showed excellent tensile strength (341.7 MPa vs. 57.0 MPa for natural wood), toughness (4.4 MJ/m3 vs. 0.4 MJ/m3 for natural wood) and Young’s modulus (24.7 GPa vs. 7.2 GPa for natural wood). Furthermore, due to low density, this material exhibited a superior specific strength of 285 MPa·cm3·g−1, which is remarkably higher than some traditional building materials, such as concrete, alloys. In addition, the cellulose scaffold was infiltrated with ANFs, which also improved the thermal stability of the hybrid material. The facile and top-down process is effective and scalable, and also allows one to fully utilize cellulose scaffolds to fabricate all kinds of advanced bio-based materials.