The short Li-C distances (Li-1-C-2 = 2.615(3) Angstrom, Li-1-C-3 = 2.644(3) Angstrom) in the X-ray crystal structure of [Li-O-C(Me)-(c-CHCH2CH2)(2)](6) (7)(6) characterize Li-cyclopropane edge coordinations. The Li-cyclopropane interactions increase the C-2-C-3 distances (1.519(3) Angstrom) relative to those of the free cyclopropyl edges (C-2-C-4 = C-6-C-7 = 1.499(2) Angstrom) by 0.02 Angstrom. The bent bonds of cyclopropane give rise to an electrostatic potential pattern, which strongly favors edge coordination as is observed experimentally in (7)(6), but also permits a metastable Li+ face complex. The cyclopropane edge also is the favored site for hydrogen bonding, but not for protonation. The C-C bond length elongations, the coordination energies E(coord), and the charge redistributions upon metal cation edge interactions all are related to the distances between the cyclopropane C-C bond centers and the cations. This is evaluated for the alkali metal cation-cyclopropane complexes (cation = Li+ to Cs+). More generally, the cyclopropane C-C bond length variations can be employed as a structural measure for the magnitudes of electrostatic interactions.