Relationship between the chain conformation in the crystal lattice and the ultimate Young's modulus has been discussed on the basis of the crystal structural information revealed by the X-ray diffraction analysis for a series of arylate polyesters with long methylene segments (-[-COC6H4CO-O(CH2)(m)O-](n)-). The X-ray structural analysis revealed that the molecular chains take the all-trans-zigzag conformations for all of the even-numbered polyesters and their model compounds as well as the odd-numbered polyesters with the methylene segmental length longer than (CH2)(14). These chain conformations have been correlated well to the ultimate Young's modulus along the chain axis or the crystallite modulus E-c, which has been estimated experimentally by the X-ray diffraction method under a constant stress and also predicted theoretically using the X-ray-analyzed crystal structures on the basis of the molecular mechanics method. The E-c was found to show the minimum at around m = 4-6 and increased gradually with an increment of m and approached the crystallite modulus of polyethylene, 235 GPa (X-ray value) similar to 316 GPa (calculate) at an infinite m value. This behavior of E-c as a function of the number of methylene segmental units m was reasonably interpreted by developing the theoretical equation of E-c for a simplified zigzag chain model composed of a repetition of two linear rods representing the benzene-ester and methylene segmental parts respectively. These findings may promise that the mechanical property of arylate polyester can be controlled by adjusting the methylene segmental length m. (C) 2014 Elsevier Ltd. All rights reserved.