  We present high-resolution (FWHM ~ 0.3-1.5 km/s) spectra of interstellar Ca I
absorption toward 30 Galactic stars. Comparisons of the column densities of Ca
I, Ca II, K I, and other species -- for individual components identified in the
line profiles and also when integrated over entire lines of sight -- yield
information on relative electron densities and depletions. There is no obvious
relationship between the ratio N(Ca I)/N(Ca II) [equal to n_e/(Gamma/alpha_r)
for photoionization equilibrium] and the fraction of hydrogen in molecular form
f(H2) (often taken to be indicative of the local density n_H). For a smaller
sample of sightlines for which the thermal pressure (n_H T) and local density
can be estimated via analysis of the C I fine-structure excitation, the average
electron density inferred from C, Na, and K (assuming photoionization
equilibrium) seems to be independent of n_H and n_H T. While the n_e obtained
from the ratio N(Ca I)/N(Ca II) is often significantly higher than the values
derived from other elements, the patterns of relative n_e derived from
different elements show both similarities and differences for different lines
of sight -- suggesting that additional processes besides photoionization and
radiative recombination commonly and significantly affect the ionization
balance of heavy elements in diffuse IS clouds. Such additional processes may
also contribute to the (apparently) larger than expected fractional ionizations
(n_e/n_H) found for some lines of sight with independent determinations of n_H.
In general, inclusion of ``grain-assisted'' recombination does reduce the
inferred n_e, but it does not reconcile the n_e estimated from different
elements. The depletion of calcium may have a much weaker dependence on density
than was suggested by earlier comparisons with CH and CN.
