Theoretical models of shockproof composite materials based on two-layer graphenes and multilayer polyvinylidene fluoride C_124H_40 + n (H–(C_2H_2F_2)_5–H) ( n = $$\overline {1,\;8} $$ ) are constructed. The electronic structure is studied using the semiempirical PM3 method that is one of version of the molecular orbital method. The orbital energies, ionization potentials, total electron energies, strength, and other properties of the considered material are calculated based on the theoretical models. The outlooks for application of these materials in the military field for manufacturing superstrong and lightweight flak jackets are considered.