1：Experimental Design and Method Selection:

Atomistic molecular dynamics (MD) simulations were performed with the Gromacs-

2：7 software package. The general AMBER force field (GAFF) was used to describe the atom types and intra- and intermolecular interaction parameters of the PDI derivatives and chloroform solvent. The atomic partial charges were optimized according to the restrained electrostatic potential (RESP) obtained at the default Hartree–Fock/6-31G* level. Sample Selection and Data Sources:

A series of bay-linked dimeric PDI derivatives with systematically changed branching position of the side alkyl chains (DPDI-C n , n = 1–5) were studied.

3：List of Experimental Equipment and Materials:

Gromacs-

4：7 software package, chloroform solvent. Experimental Procedures and Operational Workflow:

The thin-film molecular packing structures of the PDI derivatives were obtained through a series of simulations including solvent evaporation processes and thermal annealing.

5：Data Analysis Methods:

The transfer integrals for the neighboring PDI pairs were computed using a semi-empirical method based on the Zerner’s intermediate neglect of differential overlap (ZINDO) Hamiltonians. The semi-classical Marcus electron transfer theory was used to estimate the electron transfer rates between neighboring PDI units and kinetic Monte Carlo (KMC) simulations were performed to evaluate the diffusion coefficients and electron mobilities.