The unique combination of magnetic properties and structural transitions exhibited by many members of the R 5 (Si x Ge 1-x ) 4 family (R = rare earths, 0 ≤ x ≤ 1) presents numerous opportunities for these materials in advanced energy transformation applications. Past research has proven that the crystal structure and magnetic ordering of the R 5 (Si x Ge 1-x ) 4 compounds can be altered by temperature, magnetic field, pressure and the Si/Ge ratio.Results of this thesis study on the crystal structure of the Er 5 Si 4 compound have for the first time shown that the application of mechanical forces (i.e. shear stress introduced during the mechanical grinding) can also result in a structural transition from Gd 5 Si 4 -type orthorhombic to Gd 5 Si 2 Ge 2 -type monoclinic. This structural transition is reversible, moving in the opposite direction when the material is subjected to low-temperature annealing at 500 ˚C.Successful future utilization of the R 5 (Si x Ge 1-x ) 4 family in novel devices depends on a fundamental understanding of the structure-property interplay on the nanoscale level, which makes a complete understanding of the microstructure of this family especially important.Past scanning electron microscopy (SEM) observation has shown that nanometer-thin plates exist in every R 5 (Si x Ge 1-x ) 4 ("5:4") phase studied, independent of initial parent crystal structure and composition. A comprehensive electron microscopy study including SEM, energy dispersive spectroscopy (EDS), selected area diffraction (SAD), and high resolution transmission electron microscopy (HRTEM) of a selected complex 5:4 compound based on Er rather than Gd, (Er 0.9 Lu 0.1 ) 5 Si 4 , has produced data supporting the assumption that all the platelet-like features present in the R 5 (Si x Ge 1-x ) 4 family are hexagonal R 5 (Si x Ge 1-x ) 3 ("5:3")