Tunnel-coupled optically active quantum dot molecules (QDMs) have the potential to operate as spin-photon interfaces with coupled spins that interact with two different photon frequencies at the same time. A prerequisite is to deterministically prepare two (electron or hole) spins in the QDM and be able to electrically tune the orbital state couplings. Here, we demonstrate the sequential optical charging of a single QDM with two-electron spins while simultaneously maintaining the ability to widely tune orbital couplings using static electric fields and optically drive the system for quantum light generation. We optically prepare one- and two-spin states, initialize via optical pumping and explore orbital and spin relaxation dynamics for one- and two-spin states as a function of the energy detuning and hybridization of orbital states. For two-spin states, remarkably long singlet-triplet relaxation times are observed, extending beyond ∼ 100 μ s with strong dependence on the relative energy of ground and excited two-spin states. Qualitative agreement is observed with k · p calculations of phonon-mediated spin relaxation. Our results provide new quantitative understanding of the dynamics of one- and two-spin states and address a number of key prerequisites for using QDMs to create multidimensional photonic cluster states.