Quantum chemical ab initio calculations and investigations of several organic photoelectron donor, electron acceptor molecules and their supermolecules connecting via the electron insulator bridges were performed using Hartree-Fock (HF) and density functional theory (DFT) methods. The optimized ground state geometry was as initial optimizing geometry in the first excited state using ab initio configuration interaction single-excitation (CIS) method. The results of single molecule and supermolecule calculations were used for the design and ab initio calculations of two-, three-, four- and six-variable anisotropic random-walk molecular devices based on stilbene and ate-dye molecules. Two kinds of logically AND controlled molecular random-walkers were designed.