The coexistence of Li2MoO4 (LMO) and Ni0.5Zn0.5Fe2O4 (NZO) has been proven and their low‐temperature‐sintered magneto‐dielectric composites (1−x)LMO–xNZO (volume fraction factor x = 0.1, 0.3, 0.5, 0.7) were prepared by the conventional solid‐state reaction method and were sintered below 700°C. It is found that the optimal sample (x = 0.5) has good and relatively stable magneto‐dielectric performance in the frequency range from 10 MHz to 1 GHz with permittivity between 7.14 and 6.84, dielectric loss tangent between 0.09 and 0.02, and permeability between 5.23 and 3.30, magnetic loss tangent between 0.06 and 0.65, respectively. Furthermore, the verified chemical compatibility with silver indicates that the LMO–NZO ceramics are potential for low‐temperature cofired ceramic application and their multifunctional magneto‐dielectric properties also make them for potential applications in electronic devices.