Transition-metal complexes exhibit rich photochemical and photophysical behavior because they can access long-lived electronically excited states. Achieving similar functionality with first-row (3d) transition metals remains challenging and requires detailed insight into excited-state dynamics. In this contribution, computational modeling is employed to investigate how excited states evolve in time in cobalt-based molecular systems. Mixed quantum-classical non-adiabatic surface-hopping and quantum multi-layer MCTDH methods are used to describe population transfer, relaxation pathways, and long-time recovery. The results illustrate how ultrafast processes emerge from the coupled motion of electrons and nuclei and how spin-orbit coupling, vibrational motion, and structural changes shape the observed dynamics. The contribution highlights general challenges in simulating time-dependent processes in complex systems and shows how such insight is relevant for the understanding and design of light-driven processes, including emerging applications in cobalt-based photocatalysis.