A methodology combining the polarizable continuum model and optimally‐tuned range‐separated (RS) hybrid functional was proposed for the quantitative characterization of the excited‐state properties in oligoacene (from anthracene to hexacene) crystals. We show that it provides lowest vertical singlet and triplet excitation energies, singlet‐triplet gap, and exciton binding energies in very good agreement with the available experimental data. We further find that it significantly outperforms its non‐tuned RS counterpart and the widely used B3LYP functional, and even many‐body perturbation theory within the GW approximation (based on a PBE starting point). Hence, this approach provides an easily applicable and computationally efficient tool to study the excited‐state properties of organic solids of complexity. © 2017 Wiley Periodicals, Inc.