Abstract
Macroscopic fibres assembled from two-dimensional (2D) nanosheets are new and impressing type of fibre materials besides those from one-dimensional (1D) polymers, such as graphene fibres. However, the preparation and property-enhancing technologies of these fibres follow those from 1D polymers by improving the orientation along the fibre axis, leading to non-optimized microstructures and low integrated performances. Here, we show a concept of bidirectionally promoting the assembly order, making graphene fibres achieve synergistically improved mechanical and thermal properties. Concentric arrangement of graphene oxide sheets in the cross-section and alignment along fibre axis are realized by multiple shear-flow fields, which bidirectionally promotes the sheet-order of graphene sheets in solid fibres, generates densified and crystalline graphitic structures, and produces graphene fibres with ultrahigh modulus (901 GPa) and thermal conductivity (1660 W m(-1) K(-1)). We believe that the concept would enhance both scientific and technological cognition of the assembly process of 2D nanosheets.