In order to achieve optimal desalination during capacitive deionization (CDI), CDI electrodes should possess high electrical conductivity, large surface area, good wettability to water, narrow pore size distribution and efficient pathways for ion and electron transportation. In this work, we fabricated a novel CDI electrode based on a three-dimensional graphene (3DG) architecture by constructing interconnected graphene sheets with in-plane nanopores (NP-3DG). As compared to 3DG, NP-3DG features a larger specific surface area of 445 m(2) g(-1) and therefore the higher specific capacitance. The ultrahigh electrosorptive capacity of NP-3DG predicted from Langmuir isotherm is 17.1 mg g(-1) at a cell potential of 1.6 V. This can be attributed to the interconnected macropores within the graphene networks and nanopores on graphene sheets. Both of macropores and nanopores are favorable for enhancing CDI performance by buffering ions to reduce the diffusion distances from the external electrolyte to the interior surfaces and enlarging the surface area.