The molten‐salt‐mediated oxidative dehydrogenation (MM‐ODH) of ethane (C2H6) via a chemical looping scheme represents an effective carbon capture and utilization (CCU) method for the valorization of ethane‐rich shale gas and concurrent mitigation of carbon dioxide (CO2) emissions. Here, stepwise experimentation with Li2CO3‐Na2CO3‐K2CO3 (LNK) ternary salts (i) assessed how each component of the LNK mixture impacted ethane MM‐ODH performance and (ii) explored physicochemical and thermodynamic mechanisms behind melt‐induced changes to ethylene (C2H4) and carbon monoxide (CO) yields. Of fifteen screened LNK compositions, nine exhibited ethylene yields greater than 50% at 800°C while maintaining C2H4 selectivities of 85% or higher. LNK salts rich in Li2CO3 content yielded more ethylene and CO on average than their counterparts, and net CO2 capture per cycle reached a maximum of ~75%. Extended MM‐ODH cycling also demonstrated long‐term stability of a high‐performing LNK medium. Density functional theory (DFT) calculations and ab initio molecular dynamics (AIMD) simulations suggested that the molten salt does not directly activate C2H6. Meanwhile, an empirical model informed by experimental data and reaction thermodynamics adequately predicted overall MM‐ODH performance from LNK composition and provided insights into the system’s primary drivers.