AbstractThe surface porosity of graphene-based aerogels strongly influences their performance in applications involving mass transfer. However, the factors determining the surface porosities are not well-understood, hindering their application-specific optimisation. Here, through experiments and hydrodynamic simulations, we show that the high shear stress during the graphene-based aerogel fabrication process via 3D printing leads to a non-porous surface. Conversely, crosslinking of the sheets hinders flake alignment caused by shearing, resulting in a porous surface. Our findings enable fine control of surface porosity of printed graphene-oxide aerogels (GOA) through regulation of the crosslinking agents and shear stress. Using this strategy, we demonstrate the performance advantages of GOA with porous surface over their non-porous counterpart in dye adsorption, underscoring the importance of surface porosity in certain application scenarios.