One of the common obstacles in designing organic semiconductor compound is its low charge carrier mobility compared to its inorganic counterpart. Physics-based modeling and prediction methodology for such charge carrier mobility in ordered and disordered organic semiconductor materials, however, is limited to date. In this work, we present an in silico prediction scheme for charge carrier mobility in bulk organic semiconductors based on high-throughput quantum chemical methods combined with molecular dynamics simulations. Validation of the method via comparison with experimentally measured mobility values will be given for representative cases including but not limited to four organic semiconductor compounds in amorphous phase – mCP, NPB, CzC, and 2TNATA. The comparison shows potential value of the proposed methodology in ab initio mobility predictions for ordered and disordered organic semiconductor materials.