The transition to sustainable materials and eco-efficient processes in commercial electronics is a driving force in developing green electronics. Iron-catalyzed laser-induced graphitization (IC-LIG) has been demonstrated as a promising approach for rendering biomaterials electrically conductive. To optimize the IC-LIG process and fully exploit its potential for future green electronics, it is crucial to gain deeper insights into its catalyzation mechanism and structural evolution. However, this is challenging due to the rapid nature of the laser-induced graphitization process. Therefore, multiscale preparation techniques, including ultramicrotomy of the cross-sectional transition zone from precursor to fully graphitized IC-LIG electrode, are employed to virtually freeze the IC-LIG process in time. Complementary characterization is performed to generate a 3D model that integrates nanoscale findings within a mesoscopic framework. This enabled tracing the growth and migration behavior of catalytic iron nanoparticles and their role during the catalytic laser-graphitization process. A three-layered arrangement of the IC-LIG electrode is identified including a highly graphitized top layer with an interplanar spacing of 0.343 nm. The middle layer contained γ-iron nanoparticles encapsulated in graphitic shells. A comparison with catalyst-free laser graphitization approaches highlights the unique opportunities that IC-LIG offers and discuss potential applications in energy storage devices, catalysts, sensors, and beyond.