A key feature of organic pi-conjugated materials is the strong connection between their electronic and geometric structures. In particular, it has been recently demonstrated that nonlocal electron-vibration (electron-phonon) interactions, which are related to the modulation of the electronic couplings (transfer integrals) between adjacent molecules by lattice vibrations, play an important role in the charge-transport properties of organic semiconductors. Here, we use density functional theory calculations and molecular mechanics simulations to estimate the strength of these nonlocal electron-vibration couplings in oligoacene crystals as a function of molecular size from naphthalene through pentacene. The effect of each optical vibrational mode on the electronic couplings is evaluated quantitatively. The results point to a very strong coupling to both intermolecular vibrational modes and intramolecular (including high-frequency) modes in all studied systems. Importantly, our results underline that the amount of relaxation energy associated with nonlocal electron-phonon coupling decreases as the size of the molecule increases. This work establishes an original relationship between chemical structure and nonlocal vibrational coupling in the description of charge transport in organic semiconductor crystals.