Interdependence of redox state, hydrogen bonding, anion recognition and charge partition in crystals of EDT-TTF-CONHMe6Re6Se8CN6 CH3CN2CH2Cl22Electronic supplementary information (ESI) available: plot of magnetic susceptibility against temperature. See http://www.rsc.org/suppdata/cc/b3/b303416j/

Neutral π-conjugated molecules and their radical cations co-exist in EDT-TTF-CONHMe4EDT-TTF-CONHMe02 Re6Se8CN64−CH3CN2CH2Cl22whose crystal structure reveals that, upon one-electron oxidation, an activation of the N–H and C–H hydrogen bond donor ability is coupled to a deactivation of the hydrogen bond acceptor character of the carbonyl oxygen atom: this is expressed in the supramolecular hydrogen bond pattern and, ultimately, into charge localisation and partition in the solid state.