▎ 摘　　要

We report a method to introduce direct bonding between graphene platelets that enables the transformation of a multilayer chemically modified graphene (CMG) film from a paper mache-like" structure into a stiff, high strength material. On the basis of chemical/defect manipulation and recrystallization, this technique allows wide-range engineering of mechanical properties (stiffness, strength, density, and built-in stress) in ultrathin CMG films. A dramatic increase in the Young's modulus (up to 800 GPa) and enhanced strength (sustainable stress >= 1 GPa) due to cross-linking, in combination with high tensile stress, produced high-performance (quality factor of 31 000 at room temperature) radio frequency nanomechanical resonators. The ability to fine-tune intraplatelet mechanical properties through chemical modification and to locally activate direct carbon carbon bonding within carbon-based nanomaterials will transform these systems into true "materials-by-design" for nanomechanics.