Magnetic glass–ceramics based on the Li2O–Fe2O3–Al2O3–SiO2 glass system, were prepared through controlled heat treatment regimes. The effect of MO/Li2O replacements (MO=MgO, MnO, ZnO, CdO) on the crystallization process, physical and magnetic properties of the glasses and glass–ceramics were investigated. The crystalline phases formed in the glass–ceramic were lithium metasilicate (Li2SiO3), β-quartz solid solution (ss) (LiAlSi2O6), lithium ferrite (LiFe5O8), Magnesioferrite (MgFe2O4), Jacobsite (MnFe2O4), Franklinite (ZnFe2O4), lithium zinc orthosilicate (γ-Li2ZnSiO4) and lithium ferrite solid solution Li(Fe,Cd)5O8. The density of the prepared glass samples ranged from 2.69 to 2.88g/cm3, whereas the corresponding crystalline materials had a density between 2.77 to 2.95g/cm3. The microhardness of the glass samples ranged from 4665MPa to 5586MPa and increased to a range of 6268–7042MPa after crystallization. The saturation magnetization (Ms), remanence magnetization (Mr), and coercivity (Hc) of the glass–ceramics varied from 0.83 to 8.24emu/g, 0.11 to 0.97emu/g and 112 to 211G, respectively. The formation of different MFe2O4 spinel ferrite magnetic phases instead of LiFe5O8 led to a greatly enhanced saturation magnetization of the glass–ceramics. Possible use of the prepared glass–ceramics may be realized in microwave and magnetic recording applications as well as in tumors therapy.