As structural materials, crystalline or metallic glass materials have attracted scientific and practical interests. However, some mechanisms involving critical size and shear bands have adverse effects on their mechanical properties. Here, we counter these two effects by introducing a special structure with ultrafine ceramic grains (with a diameter of ∼2.0 nm) embedded into a metallic glass matrix, wherein the grains are mainly composed of a Ta-W-N solid solution structure in nature, surrounded by a W-based amorphous matrix that contains Ta and N atoms. Such a structure is in situ formed during preparation, which combines the merits of both phases to achieve simultaneous increase in hardness and toughness relative to references (pure TaN and W) and thus superior wear resistance. Even more remarkable, a favorable variation of increased hardness but reduced elasticity modulus can be induced by this structure. Intrinsically, ultrafine ceramic grains (free of dislocations), embedded in the metallic glass matrix, could prevent shear band propagation within the glass matrix and further improve the hardness of the matrix material. In return, such glass matrix allows for stiffness neutralization and structural relaxation to reduce the elasticity modulus of ceramic grains. This study will offer a new guidance to fabricate ultrahigh-performance metal-based composites.