Crater-like architectural aluminum current collectors is prepared by a simple chemical etching method with NaOH-based solutions, and investigate the effect of aluminum surface morphology on its electrochemical performance as cathode current collector in Li-ion batteries. Characterization data reveal an acceptable tensile strength and surface hydrophilicity in the etched aluminum current collector, together with the creation of a rough surface with many reticular crater-like pits. In Li-ion cells using LiCoO2 as the active material, the crater-like architectural aluminum foil is electrochemically stable as the current collector, when in contact with other cell components during the charge–discharge processes. The improved electrochemical performance is attributed to the good electrical contact between cathode material particles and the current collector, and the resulting efficient electron transfer.