The effect of isoelectronic substitution within single crystals of (Sr1−xCax)2−yIrO4+z is explored. The nominal n = 1 Ruddlesden-Popper phase with y = 0, z = 0 remains stable from x = 0 until x = 0.11, where the antiferromagnet spin-orbit Mott insulating state persists. An increase in the saturated moment is observed with increasing Ca-substitution, suggesting a modified coupling of the in-plane moments relative to the in-plane rotation of IrO6 octahedra. Beyond x = 0.11, the x = 1/4, y = 0, z = 1/2 structural phase Sr3CaIr2O9, consisting of a three-dimensional network of corner sharing octahedra, begins to intermix and eventually nucleates phase pure crystals at higher starting Ca-content. An insulating, nonmagnetic ground state is observed in this phase attributable to the J = 0 state and is consistent with a recent powder study. At higher Ca-concentrations beyond x = 0.75, crystals begin to stabilize in the y = 1/3, z = 0 quasi one-dimensional Ca5Ir3O12 structure. The low temperature transport in this chain-based structure is well described via variable range hopping, and an antiferromagnetic ordering transition appears below TN = 9 K. Our data provide a detailed mapping of the electronic and structural properties accessible as the structural framework of the canonical spin orbit Mott insulator Sr2IrO4 is destabilized via isovalent chemical substitution.