Alternative information-theoretic (IT) measures of the chemical bond multiplicity and its covalent/ionic composition in the orbital communication theory (OCT) are examined using Shull’s natural orbital (NO) model of the homopolar bond in . In OCT a molecule is treated as an information (probability-scattering) system, generated by the network of conditional probabilities (from the quantum mechanical superposition principle) linking elementary events of the adopted perspective. For the first time this atomic orbital (AO) invariant, two -NO description of Shull allows one to examine in several alternative representations the behavior of the previously adopted IT indices, of the channel average communication noise (OCT-covalency) and infor- mation flow (OCT-ionicity), with changing internuclear distance R , from the united atom (R=0) to the separated atoms limit (SAL) (R→∞) . The adopted references include the two -electron atomic and ionic functions of the model, as well as the alter- native one -electron functions, of the AO and NO sets, respectively. The numerical results for the Wang function description of are reported and a general agreement with the accepted chemical intuition is tested. Joint probabilities of Shull’s reference states are linked to the energy partitioning. The incorrect SAL behavior of the OCT- ionicity index, giving rise to the constant (interaction independent) overall multiplicity measure, emphasizes a need for a revision of these IT bond descriptors. The modified set of indices is proposed, reflecting the complementary localization (determinicity) and delocalization (indeterminicity) aspects of the communication system in question.