Zn–MnO₂ alkaline batteries have been the dominant primary energy storage solution for decades. Despite their success, there is a desire to improve their discharge capacity and energy density as they approach their practical engineering limits. Since the capacity of alkaline batteries is limited by the Zn anode mass, one possible pathway to enhance the energy density is to modify the Zn anode with secondary materials that boost their capacity without sacrificing their stability. Herein, partial deployment of Al in Zn anodes was investigated to increase capacity and energy density as Al has a ~3.5 fold higher theoretical gravimetric capacity than Zn. To do that, Zn-rich electrolytic Zn/Al (e-Zn/Al) was synthesized, physically characterized and exposed to a series of electrochemical methods in both three-electrode cells and cylindrical full cells, including linear sweep and cyclic voltammetry, electrochemical impedance spectroscopy, and charge/discharge cycling. In addition, an electrochemical quartz crystal microbalance was utilized to explore the influence of ZnO and Al(OH)₃ electrolyte additives to KOH on Zn corrosion and passivation. It was shown that partial Al inclusion significantly improved capacity, to 581 mAh g⁻¹_anode (~784 Wh kg⁻¹_anode) at C/20. Finally, excellent cycle performance was observed over 800 h in secondary full cells.