The Young＇s modulus or crystallite modulus of ca. 10 GPa has been obtained experimentally by the X-ray diffraction method for isotactic poly(methyl methacrylate) (it-PMMA) crystal along the chain direction. The modulus, calculated by the energy minimization method, for the double-stranded helix model of it-PMMA was 19 GPa, which was about twice as high as that of the single helix model, 11 GPa. This calculation indicated clearly a role for the intertwining of the two chains on the mechanical toughening of the polymer crystal along the chain axis, although the calculated value was an overestimation compared with the observed value.