Formation of a partially charge-transfer or partially oxidized/reduced state has been one of the most important requirements for the development of highly conducting molecular materials, such as organic metals and superconductors. This requirement has been fulfilled by combining appropriate electron-donor and acceptor molecules to construct multi-component molecular complexes/salts, such as (TTF+0.59)(TCNQ-0.59) and (BEDT-TTF+0.5)2X-, where TTF = tetrathiafulvalene, TCNQ = tetracyanoquinodimethane, BEDT-TTF = bis(ethylenedithio)tetrathiafulvalene, and X = monovalent inorganic anion. Here, we propose a methodology to fulfill this requirement by a single neutral molecule; namely, we have connected two TTF+0.5-type partially oxidized π-skeletons through a boron anion to design a purely organic zwitterionic neutral radical {[(PDT-TTF-Cat)2]+B-}•. This molecule was successfully obtained as air-stable crystals containing solvent tetrahydrofuran (THF) molecules. Measurements of electrical resistivity, magnetic susceptibility, and X-ray diffraction reveal that the partially oxidized state is certainly formed, which enables realization of a 3/4-filled electron band. Furthermore, this system has intramolecular charge degrees of freedom, attributable to the two TTF+0.5 π-skeletons introduced into the molecule. The resulting interplay of intra- and intermolecular charge degrees of freedom (or simply, intra- and intermolecular electronic interactions) has led to multi-step phase transitions and crossover, providing unique strongly correlated electron properties, such as the formation of a three-dimensional charge-ordered dimer-Mott insulating state and its melting triggered by disorder-order transformation of the co-crystallized solvent THF molecules at low temperatures.