^ These authors contributed equally ABSTRACT: Here we demonstrate that liquid phase exfoliation can be used to convert layered crystals of nickel hydroxide into Ni(OH) 2 nanosheets in relatively large quantities and without the need for ion intercalation. While other procedures require harsh synthesis conditions and multiple reaction steps, this method involves ultrasonication of commercially available powders in aqueous surfactant solutions and so is relatively mild and potentially scalable. Such mild exfoliation is possible because the surface energy of Ni(OH) 2 , as measured by inverse gas chromatography, is relatively low at ~70 mJ/m 2 , similar to other layered materials. TEM, AFM, XPS and Raman spectroscopy show the exfoliated nanosheets to be relatively thin (mean ~10 monolayers thick) and of good quality. Size selection by liquid cascade centrifugation allowed the production of samples with mean nanosheet lengths ranging from 55 to 195 nm. Optical measurements on dispersions showed the optical absorption coefficient spectra to be relatively invariant with nanosheet size while the scattering coefficient spectra varied strongly with size. The resultant size-dependence allows the extinction spectra to be used to estimate nanosheet size as well as concentration. We used the exfoliated nanosheets to prepare thin film electrodes for use in supercapacitors and as oxygen evolution catalysts. While the resultant capacitance was reasonably high at ~1200 F/cm 3 (20 mV/s), the catalytic performance was exceptional with currents of 10 mA/cm 2 observed at overpotentials as low as 297 mV, close to the state of the art.Recently, an alternative approach, 19, 24 called liquid phase exfoliation (LPE), 25 has been developed to exfoliate uncharged layered crystals (i.e. those without interlayer ions) to give liquid-dispersed nanosheets. This method involves the production of few-layer nanosheets by shearing 26 or ultrasonication 20 of layered crystals in appropriate stabilising liquids (i.e. certain solvents 27 and surfactant 28 or polymer solutions 29 ). In each case, interactions between the stabilising liquid and the nanosheet surface reduce the net exfoliation energy and stabilise the nanosheets against aggregation. 24 The resultant 23 standard Ni(OH) 2 dispersion (C i = 20gL -1 , C surf = 9g L -1 , t sonic = 4h, f = 1.5krpm, t cf = 120min). C) AFM data for nanosheet length plotted versus nanosheet thickness for a standard Ni(OH) 2 dispersion. The dashed line represents L=10N. Inset: Sample AFM image. D) Histogram of nanosheet thicknesses, N, as measured by AFM. The line represents a lognormal distribution. Inset: Magnified image of low N portion of histogram. E) Optical extinction, absorption, and scattering spectra of Ni(OH) 2 in surfactant solution. Inset: magnified view showing absorption spectrum. F) Final Ni(OH) 2 nanosheet concentration plotted against surfactant concentration showing a peak at ~10g L -1 of sodium cholate. The dispersions in 1F were prepared with initial powder concentration C i = 10g L -1 , t soni...