The response of micrometric pseudo-single crystals of β-H2NiO2, deposited on an Au substrate and submitted to high rate charge/discharge cycling under controlled current conditions, is studied by in situ μ-Raman spectroscopy. The intensities of the Raman background and of the hydroxyl stretching band are used to probe in time the single-particle surface and bulk oxidation states respectively. Results, obtained in the absence of electrical binders and chemical dopants, substantiate previous electrochemical investigations suggesting that the occurrence of the nickel electrode activation process is related to the formation of a thin surface limiting layer hindering the active material capacity to store and deliver energy. The feasibility of in situ μ-Raman spectroscopy on nickel hydroxide single particles submitted to electrochemical operation is demonstrated for the first time.