This paper reports a pH-mediated hydrothermal reduction method that combines with moulding methods, allowing controllable fabrication of high density (up to 1.6 g cm−3) isotropic graphene macrostructures with various shapes. This “graphene” (CG) has a compressive strength of 361 MPa (6 times higher than conventional graphite products) and electrical conductivity of 7.6 S cm−1. The processing steps are scalable.