We have investigated the electronic structure of meta-stable perovskite Ca(1 - x)Sr(x)IrO(3)(x = 0, 0.5, and 1) thin films using transport measurements, optical spectroscopy, and first-principles calculations. We artificially fabricated the perovskite phase of Ca(1 - x)Sr(x)IrO(3), which has a hexagonal or post-perovskite crystal structure in bulk form, by growing epitaxial thin films on perovskite GdScO(3) substrates using an epi-stabilization technique. The transport properties of the perovskite Ca(1 - x)Sr(x)IrO(3) films systematically change from nearly insulating (or semi-metallic) for x = 0 to weakly metallic for x = 1. Due to the extended wavefunctions, 5d electrons are usually delocalized. However, the strong spin-orbit coupling in Ca(1 - x)Sr(x)IrO(3) results in the formation of effective total angular momentum J(eff) = 1/2 and 3/2 states, which puts Ca(1 - x)Sr(x)IrO(3) in the vicinity of a metal-insulator phase boundary. As a result, the electrical properties of the Ca(1 - x)Sr(x)IrO(3) films are found to be sensitive to x and strain.