Lithium‐aluminum alloy electrodes have shown a great deal of promise for meeting the performance requirements of negative electrodes in batteries for off‐peak energy storage in utility networks and for vehicle propulsion. To develop negative electrodes that meet the cell performance goals, the effects of a number of variables on the lithium‐aluminum electrode performance were determined. Investigations were conducted to determine the effects of volume fraction electrolyte in the electrode, electrode thickness, fabrication technique, lithium concentration in the Li‐Al alloy, and current collector in the electrode. Electrochemically formed Li‐Al electrodes that are 0.32 cm thick, have an electrolyte volume fraction of 0.2 in the charged state, and contain about 2 weight percent stainless steel wire current collector have demonstrated the performance goals for the negative electrodes in a electric automobile battery. For electrode thicknesses ≥0.64 cm, vibratorily loaded pyrometallurgical Li‐Al electrodes with porous metallic current collectors have demonstrated the highest lithium utilization and capacity density over a wide range of discharge current densities and have met the performance goals for negative electrodes in a off‐peak energy storage battery.