Graphene-based papers attract particular interests recently owing to their outstanding properties, the key of which is their layer-by-layer hierarchical structures similar to the biomaterials such as bone, teeth and nacre, combining intralayer strong sp2 bonds and interlayer crosslinks for efficient load transfer. Here we firstly study the mechanical properties of various interlayer and intralayer crosslinks via first-principles calculations and then perform continuum model analysis for the overall mechanical properties of graphene-based papers. We find that there is a characteristic length scale l_{0}, defined as \Sqrt{Dh_{0}/4G}, where D is the stiffness of the graphene sheet, h_{0} and G are the height of interlayer crosslink and shear modulus respectively. When the size of the graphene sheets exceeds 3l_{0}, the tension-shear (TS) chain model that are widely used for nanocomposites fails to predict the overall mechanical properties of the graphene-based papers. Instead we proposed here a deformable tension-shear (DTS) model by considering the elastic deformation of the graphene sheets, also the interlayer and intralayer crosslinks. The DTS is then applied to predict the mechanics of graphene-based paper materials under tensile loading. According to the results we thus obtain, optimal design strategies are provided for designing graphene papers with ultrahigh stiffness, strength and toughness.

23 pages, 6 figures