Dual‐salt magnesium/lithium‐ion batteries (MLIBs) benefit from fast lithium ion diffusion on the cathode side while providing safety due to the dendrite‐free Mg2+ stripping/plating mechanism on the anode side. Bulk MoS2 (B‐MoS2), as a cathode for magnesium‐ion batteries (MIBs), suffers from low conductivity and relatively van der Waals gaps and, consequently, resists against divalent Mg2+ insertion due to the high Coulombic interactions. In MLIBs, it exhibits a Daniell‐cell type mechanism with the sole accommodation of Li+. In this paper, the synthesis of a 1T/2H mixed‐phase MoS2(MP‐MoS2) modified with a hyperbranched polyethylene ionomer, I@MP‐MoS2, for high‐capacity MLIBs with a distinct Mg2+/Li+ co‐intercalation mechanism is reported. Benefiting from the enhanced conductivity (due to 53% metallic 1T phase), expanded van der Waals gaps (79% expansion compared to B‐MoS2, 1.11 vs 0.62 nm), and enhanced interactions with THF‐based electrolytes following the modification, I@MP‐MoS2 shows a dramatically increased Mg2+ storage compared to its parent analogue (144 mAh g−1 vs ≈2 mAh g−1 at 20 mA g−1). In MLIBs, I@MP‐MoS2 is demonstrated to exhibit remarkable specific capacities up to ≈270 mAh g−1 at 20 mA g−1 through a Mg2+/Li+ co‐intercalation mechanism with 87% of capacity retention over 200 cycles at 100 mA g−1.