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Iridium-based members of the Ruddlesden-Popper family of oxide compounds are characterized by a unique combination of energetically comparable effects: crystal-field splitting, spin-orbit coupling, and electron-electron interactions are all present, and the combine to produce a Jeff = 1/2 ground state. In the bilayer member of this series, Sr3Ir2O7, this state manifests as electrically insulating, with unpaired Ir4+ spins aligned along the long axis of the unit cell to produce a G-type antiferromagnet with an ordered moment of 0.36 uB. In this work, this Mott state is destabilized by electron doping via La3+ substitution on the Sr-site to produce (Sr1−x Lax)3Ir2O7. The introduction of carriers initially causes nano-scale phase-separated regions to develop before driving a global insulator-to-metal transition at x=0.04. Coinciding with this transition is the disappearance of evidence of magnetic order in the system in either bulk magnetization or magnetic scattering experiments. The doping also enhances a structural order parameter observed in the parent compound at forbidden reciprocal lattice vectors. A more complete structural solution is proposed to account for this previously unresolved distortion, and also offers an explanation as to the anomalous net ferromagnetism seen prior in bulk measurements. Finally, spin dynamics are probed via a resonant x-ray technique to reveal evidence of spin-dimer-like behavior dominated by inter-plane interactions. This result supports a bond-operator treatment of the interaction Hamiltonian, and also explains the doping dependence of high temperature magnetic susceptibility.