Covellite phase CuS and carrollite phase CuCo2S4 nano-and microstructures were synthesized from tetrachloridometallate-based ionic liquid precursors using a novel, facile, and highly controllable hot -injection synthesis strategy. The synthesis parameters including reaction time and temperature were fir st optimized to produce CuS with a well-controlled and unique morphology providing the best electrocatalytic activity towards the oxygen evolution reaction (OER). In an extension to this approach, the electrocatalytic activity was further improved by incorporating Co in the CuS synthesis method to yield CuCo2S4 microflowers synthesized via the same approach. Both routes provide high microflower yields of >80 wt.%. The CuCo 2S4 microflowers exhibit a superior performance for the OER in alkaline medium compared to CuS. This is demonstrated by a lower onset potential (~1.45 V vs. RHE @10 mA/cm 2 ), better durability, and higher turnover frequencies compared to bare CuS flowers or commercial Pt/C and IrO2 electrodes. Likely, this effect is a associated with the presence of Co 3+ sites on which a better adsorption of reactive species formed during OER (e.g., OH, O, OOH, etc.) can be achieved, thus reducing the OER charge transfer resistance, as indicated from XPS and EIS measurements.