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Some triphenyltin(IV) adducts with a family of diphosphoryl ligands, RR 0 P(O)-X-P(O)RR 0 (R ¼ OPh, Ph, R 0 ¼ R, An (aniline)) and X ¼ 1,4-OC 6 H 4 O, 1,4-OC 6 H 4 NH, 1,4-NHC 6 H 4 NH 1,4-(NHCH 2 ) 2 C 6 H 4 , 1,3-(NHCH 2 ) 2 C 6 H 4 and piperazine have been synthesized and characterized by IR and NMR spectroscopy. X-Ray crystallography reveals that the structure of these complexes comprises a binuclear arrangement with two SnPh 3 Cl moieties linked via the bridging P(O)-X-P(O) ligands. The influence of the ligand structures on the organization of the crystal structures and the coordination interactions are discussed. Studies of the crystal packing reveal NH/Cl, CH/Cl or CH/O hydrogen bonding interactions, as a function of the X or R groups, to be the main factor controlling the supramolecular architecture in this series of complexes. Based on the results from quantum theory of atoms in molecules (QTAIM) and natural bond orbital (NBO) analyses, Sn-ligand interactions are found to be mainly electrostatic (donor-acceptor-like with charge transfer from the phosphoryl donors to the tin atoms). The stronger coordination bonds are found in the complexes containing Ph substituents with aliphatic spacers, in agreement with the experimental evidence. Binuclear arrangements instead of polymeric or chelating systems may be attributed to the steric demands of SnPh 3 Cl, regardless of the ligand structures. † Electronic supplementary information (ESI) available: The crystal data and the details of the X-ray analysis, selected bond lengths, bond angles, hydrogen bonding data for the ligand 6Ph and computational data for fully optimized structures. CCDC 990940-990945. For ESI and crystallographic data in CIF or other electronic format see