In this study, Zn-Al ferrite/polypyrrole (PPy) nanocomposites were synthesized and thoroughly characterized to explore their potential for microwave applications. X-ray diffraction analysis confirmed the presence of ZnO, AlFeO3, and Fe2O3 phases, with the crystal size decreasing from 31 nm to 19.6 nm as aluminum content increased. High-resolution transmission electron microscopy (HR-TEM) revealed a distinctive core–shell morphology, where the polypyrrole encapsulates the ZnAlxFe2−xO4 particles. Magnetic measurements showed that decreasing aluminum concentration led to a reduction in both saturation magnetization (Ms) from 75 emu/g to 36 emu/g and remanent magnetization (Mr) from 2.26 emu/g to 2.00 emu/g. Dielectric analysis indicated that both the real (ε′) and imaginary (ε″) components of dielectric permittivity decreased with increasing frequency, particularly between 10 and 14 GHz. Furthermore, electrical modulus analysis highlighted the significant impact of aluminum doping on relaxation time (τIP), indicating the presence of interface polarization. Impedance spectroscopy results underscored the dominance of interface polarization at lower frequencies and the presence of strong conduction paths at higher frequencies. These combined magnetic and dielectric loss mechanisms suggest that the Zn-Al ferrite/polypyrrole nanocomposite is a promising candidate for advanced microwave absorption applications.