of OGF can be transformed from hydrophobic to hydrophilic. Meanwhile, its surface wettability can be reversibly switched and the imbibition rate can be readily modulated by controlling the applied potential. Thanks to its large pore sizes and much less tortuous channels (Figure 1b), this OGF showed an extremely high dynamic rate of imbibition (3.0 mg s −1/2 mm −2 ) at −0.9 V. This value is more than triple those of the graphene foam with a disordered pore structure (DGF, 0.89 mg s −1/2 mm −2 ) and CNT sponge (0.80 mg s −1/2 mm −2 ) at the same potential. [48] The average imbibition rate of OGF (0.347 mg s −1 mm −2 ) is even 100 times larger than that of the switchable imbiber made of porous Au sponge (3.5 µg s −1 mm −2 ). [47] OGF and DGF were prepared via our previously reported methods [49,50] followed by thermal annealing at 900 °C under Ar protection (see the Experimental Section). X-ray photoelectron spectral (XPS) examinations indicated that the atomic content of oxygen for GO was about 30%, and it decreased to 3.5% for OGF or 4.2% for DGF ( Figure S2, Supporting Information). In the C1s XPS spectrum of GO, the areal ratio of the peaks associated with intact and oxidized carbons (A CC /A OC ) [50][51][52] was measured to be 0.71, and it was increased to 24.7 for OGF and 20.4 for DGF ( Figure S3, Supporting Information). These results demonstrate that the oxygen-containing groups of GO were mostly eliminated by hydrothermal reduction and thermal annealing. The infrared (IR) spectra of OGF and DGF also do not show any peaks related to functional groups ( Figure S4, Supporting Information). Additionally, the intensity of breathing vibration of benzene rings at 1580 cm −1 was weakened after thermal treatment, reflecting that the molecular structure became more symmetric upon the partial recovery of conjugated domains. [53][54][55] The intensity ratio of the Raman D-(≈1340 cm −1 ) and G-bands (≈1585 cm −1 ) was increased from 0.98 for GO to 1.28 and 1.39 for OGF and DGF ( Figure S5, Supporting Information), also confirming the partial restoration of conjugated structure to form small graphene domains. [56,57] The cross-section and side-view scanning electron microscopy (SEM) images of OGF showed its highly oriented porous microstructure, and the thermal annealing at 900 °C induced negligible change in its morphology (Figure 2, and Figures S6−S11, Supporting Information). [49] The graphene walls interconnected with each other, and most of them were perpendicular to the cross section of OGF from its bottom to top ( Figure S8, Supporting Information), while a few graphene layers lay vertical to oriented channels (Figures S10 and S11, Supporting Information). The average radius of the pores was measured to be about 12.5 µm. For comparison, DGF showed a much more disordered microporous structure. The arrangements of graphene walls are completely random. Meanwhile, the distribution of pore sizes is broad with an average radius of only 4.9 µm.Graphene foam is a porous material constructed by 2D graphene sheets to form ...