Cobalt oxide thin films have been deposited with remote plasma atomic layer deposition (ALD) within a wide temperature window (100–400°C), using CoCp2 as cobalt precursor and with a remote O2 plasma as oxidant source. The growth rate was relatively high at 0.05nm per ALD-cycle and resulted in the deposition of high density (∼5.8gcm−3), stoichiometric Co3O4. For the electrochemical analyses, Co3O4 was deposited on a Si substrate covered with an ALD-synthesized TiN layer to prevent Li diffusion. The as-deposited electrodes were investigated in a three-electrode electrochemical cell using constant current (CC) charge/discharge cycling and Galvanostatic Intermittent Titration Technique (GITT) in combination with Electrochemical Impedance Spectroscopy (EIS). Compared to the literature, ALD-deposited Co3O4 exhibited a high electrochemical activity (∼1000mAhg−1) and the formation of a solid electrolyte interface has been identified by EIS.