The relative binding energies of a series of pyridyl ligand/metal complexes of the type [(ML2)-L-I](+) and [(ML3)-L-II](2+) are investigated by using energy-variable collisionally activated dissociation in a quadrupole ion trap mass spectrometer. The pyridyl ligands include 1,10-phenanthroline and various alkylated analogues, 2,2'-bipyridine, 4,4'-dimethyl-2,2 -bipyridine, and 2,2':6',2 " -terpyridine, and the metal ions include cobalt, nickel, copper, zinc, cadmium, calcium, magnesium, lithium, sodium, potassium, rubidium, and cesium. The effect of the ionic size and electronic nature Of the metal ion and the polarizability and degree of preorganization of the pyridyl ligands on the threshold activation voltages, and thus the relative binding energies of the complexes, are evaluated. Correlations are found between the binding constants of [(ML3)-L-II](2+) Complexes in aqueous solution and the threshold activation voltages of the analogous gas-phase complexes determined by collisionally activated dissociation.