has attracted attention due to its fascinating properties such as high carrier mobility, [ 6–8 ] high thermal conductivity, [ 9 , 10 ] extraordinary elasticity and stiffness [ 11 ] and other properties. While mechanical exfoliation, [ 6 ] liquid exfoliation, [ 12 ] and epitaxial growth [ 13 ] can produce pristine graphene, graphene yields are currently too low for large-scale production of macrostructures. In contrast, chemical reduction of graphene oxide provides ‘graphene’ sheets in large scale for graphene macrostructures. [ 14–16 ] Graphene-based macrostructures prepared to date have been relatively weak mechanically, given their fl exible and often relatively porous or open structures, [ 17–26 ] particularly with respect to compressive strength when compared with commercial graphite products. [ 27–29 ] Achieving highly compacted and thus “fully dense” macrostructures based on graphene and measuring the physical properties of such material(s) is thus an important goal. Here, we report a pH-mediated hydrothermal reduction which is combined with moulding methods and allows controllable fabrication of compact high density graphene macrostructures with various shapes. The compact graphene (CG) product that is fabricated in this study shows great advantages over hitherto reported 3-D graphene products, [ 17–26 ] e.g. , a solid microstructure and a high density ( ∼ 1.6 g cm − 3 ) which is comparable to conventional graphite products [ 27–29 ] and an ultrahigh compressive strength ( ∼ 361 Mpa) which is 6 times higher than