Lithium sulfur (Li-S) batteries are considered one of the most promising energy storage devices due to their high specific capacity, pollution-free reactant, and low cost. However, the “shuttle effect” of lithium polysulfide (Li2S
x
) leads to a fast capacity decay and poor cycle life. Here, the magnetorheological effect (MRE) is first applied in Li-S batteries and a magnetic control electrolyte is designed by introducing carbonyl iron powders (CIPs) to improve the performance of Li-S batteries. According to adsorption bonding theory, the binding energy of Fe site with Li2S4 is up to 2.68 eV via discrete Fourier transform (DFT) calculation. After coupling an external magnetic field, the uniform distribution of CIPs avoids the accumulation on the cathode surface. The induced magnetic field of spherical particles captures dissolved S
x
2− effectively by Lorenz force, which is confirmed by adsorption experiments. These magnetized particles form a magnetic shield layer in the electrolyte and alleviate the “shuttle effect.” At 0.2 C, the initial specific capacity reaches 1296 mAh g−1. Magnetic control electrolyte provides not only a novel insight but also creates a new possibility for mitigating the “shuttle effect” thereby promoting performance of Li-S batteries.