Primary aluminium production is energy- and GHG-intensive in which electrolysis is by far the most energy- and GHG-intensive process. This paper’s aim is to study the effects on (1) primary energy use, (2) GHG emissions and (3) energy and CO2 costs when energy end-use efficiency measures are implemented in the electrolysis. Significant savings in final and primary energy use, GHG emissions and energy and CO2 costs can be achieved by implementing the studied measures. Vertical electrode cells and the combination of inert anodes and wettable cathodes are among the measures with the highest savings in all three areas (primary energy use, GHG emissions and energy and CO2 costs). Direct carbothermic reduction is one of the measures with the highest savings in primary energy use and energy and CO2 costs. For GHG emissions, direct carbothermic reduction is the more beneficial choice in regions with a high proportion of coal power, while inert anodes are the more beneficial choice in regions with a high proportion of low-carbon electricity. Although a company potentially can save more money by implementing the direct carbothermic reduction, the company should consider implementing the vertical electrode cells together with other energy-saving technologies since this would yield the largest GHG emission savings while providing similar cost savings as the direct carbothermic reduction. It may be necessary to impose a price on GHG emissions in order to make inert anodes cost-effective on their own, although further evaluations are needed in this regard. There is a potential to achieve carbon-neutrality in the reduction of aluminium oxide to pure aluminium.