Iron & steel (I&S) and aluminum (Al) manufacturing are energy- and GHG-emissions intensive, and considered among the most difficult-to-decarbonize sectors. The project seeks to develop sustainable power-to-gas (PtG)-based strategies driven by competitively priced low-carbon electricity toward the decarbonization of these industries, focusing on direct reduction of iron (DRI)-electric arc furnace (EAF) I&S processes and alumina refining calcination processes. These strategies will enable switching from natural gas to electrolytic hydrogen and synthetic natural gas (SNG) to supply process heat, reducing agents and electricity. Tailored PtG processes will be developed and integrated with I&S/Al processes, while minimizing changes in process equipment and cost. Oxyfuel combustion processes will also be integrated to efficiently and affordably sink and recycle CO2 for SNG synthesis, in conjunction with waste energy/material utilization. The integrated PtG-I&S/Al processes will be thermodynamically, economically, and environmentally evaluated and optimized, and benchmarked with existing industrial and alternative decarbonization (carbon capture) approaches.