This thesis describes research on magnetism, structure, and vibrational dynamics in a number of magnetic and non-magnetic nanoscaled heterostructures. Much attention is paid to a thorough structural characterization of the materials, because this is essential for understanding the stabilization of metastable phases (here: fcc-like Fe and alpha-Sn), magnetic properties such as anisotropy and magneto-volume instabilities, or lattice vibrational behavior. A number of experimental techniques were used, such as 57Fe and 119Sn Conversion Electron Mössbauer Spectroscopy (CEMS), Magneto-Optic Kerr Effect (MOKE), 119Sn Nuclear Resonant Inelastic X-ray Scattering (NRIXS), X-Ray Diffraction (XRD), Reflection High Energy Electron Diffraction (RHEED), Low Energy Electron Diffraction (LEED), and Auger Electron Spectroscopy (AES).