Leather, as a kind of renewable biomass, is naturally rich in dipoles as well as excellent 3D fiber structure, which provides the possibility for its application in electromagnetic shielding field. This study combined the utilization of chromium-containing wastewater with the intelligent development of leather. Nano zero-valent iron (NZVI) was innovatively used to prepare magnetic Mg/Fe/Cr layered double hydroxide (MgFeCr-LDHs) by co-precipitation method while treating chromium wastewater. And magnetic MgFeCr-LDHs was used for tanning leather, which prepared electromagnetic shield leather (MgFeCr-LDHs/L). Fe3+ and Cr3+ in MgFeCr-LDHs were closely bonded with the active groups on collagen fibers by chemical bonding, which give leather hygrothermal stability. The shrinkage temperature of MgFeCr-LDHs/L reached 89.1°C. Electromagnetic shielding efficiency of magnetic MgFeCr-LDHs/L reached 25 dB due to MgFeCr-LDHs had better dielectric and magnetic losses to electromagnetic waves. Magnetic MgFeCr-LDHs/L also had good softness and mechanical properties. In summary, we expect magnetic MgFeCr-LDHs/L to be used as a wearable material in the field of electromagnetic shielding.