The brittleness of bioglass/ceramics limits their applications in bone repair. The toughness of the glass matrix can be enhanced by adding nanoscale reinforcements at random; however, the effect is quite limited. This study proposes a novel strategy to prepare controllable fabricating lamellar precursors with multiwalled carbon nanotubes (MWCNTs) film/glass/MWCNTs film sandwich structure by a high-temperature foaming method. Subsequently, the precursor was sintered by spark plasma to obtain a composite material with strong cross-linking between MWCNTs and the glass matrix. The mechanical properties of the composites were characterized, and mechanisms were analyzed by the finite element method. The results revealed that the glass composite with 1.0 wt% MWCNTs had a significantly enhanced fracture toughness (2.65 MPa m1/2) and flexural strength (145 MPa), which were 2.1 times and 1.8 times higher than those of pure glass, respectively. This increase in toughness is attributed to the strong resistance of the well-combined bent and entangled MWCNTs to the fiber pull-out process. The glass/MWCNTs composite showed a low electrical resistivity of 5.8 Ω cm, which would aid skeletal restoration. Thus, this strategy paves a facile way to prepare the highly toughed bio-glass with multifunctional properties.