Now considerable attention should be placed for the search of high-performance air-stable organic semiconductor materials (OSCMs) to fulfill the meet of applications. Crystal structure prediction (CSP) is a powerful tool to predict the CT properties of OSCMs. In this paper, using a new combined QM and MM method, the packing motifs of the experimental and the other possible polymorphisms of TIPS-PEN and TIPS-TBT were successful predicted. Here, we successfully predicted their charge transport properties with nothing more than the molecular geometry as the starting point and provide a rational method in designing of OSCMs.