Magnetic ordering in materials that do not have partially filled d or f orbitals is a topic of interest in recent years. The presence of defects can break lattice symmetry, modify the energy landscape, and create quantum confinement, inter-layer interactions in layered solids leading to fascinating properties different from the ideal 2D sheets. In this chapter, defect-induced magnetic ordering in fullerene thin films and 2D transition metal dichalcogenide MoS2 are discussed. It was found that energetic proton beams can induce magnetic ordering in C60 films and MoS2, and in the case of MoS2 the magnetization displays a Curie temperature above room temperature.