Young’s modulus E for polyethylene in the chain direction is calculated with molecular orbital theory applied to n-alkanes C3H8, through n-C13H28 and analyzed with the cluster difference method. Semiempirical CNDO, MNDO, and AM1 models and ab initio HF/STO-3G, HF/6-31G, HF/6-31G*, and MP2/6-31G* models are used. Cluster-difference results, when extrapolated to infinite chain length, give E in good agreement with moduli evaluated with molecular cluster or crystal orbital methods, provided minimal basis sets are employed. E decreases from 495 GPa (CNDO) to 336 GPa (MP2/6-31G*) as the level of theory is improved, consistent with established behaviors of the various models. Our calculations do not reproduce earlier molecular cluster or crystal orbital results, which gave E < 330 GPa. The most rigorous MP2/6-31G* model is known to overestimate force constants by similar to 11%; the scaled modulus E = 299 GPa is in good accord with E = 306 GPa from recent calculations based on experimental vibration frequencies.