The nanocomposite Fe-A/SiO2 soft magnetic materials, with Cu, Ni, and Fe2O3 as dopants, were produced using a mechanical alloying technique. Our central objective was to explore the impact of process parameters on Fe/SiO2 nanocomposite properties. We assessed varying milling time and dopant addition rates, analyzing structural, morphological, and magnetic aspects through SEM, EDS, XRD, and VSM at different synthesis stages. The XRD pattern revealed iron, Fe(Ni), Fe(Cu), and Fe2O3 with an average crystallite size of 28–39 nm and lattice strain of 0.0097%–0.0222%. Notably, the lattice parameters decreased from 0.2852 to 0.2836 nm. Among nanocomposites, FeCu/SiO2 displayed the smallest crystallite size (34.3 nm), while FeNiSiO2 showed the highest lattice parameter (0.2853 nm). The ATR analysis unveiled Si–O–Si stretching vibrations at 1052 cm−1, intensifying with milling time. The inclusion of Cu and Ni in the FeSiO2 system significantly influenced the Si–O–Si bond. Coercivity and remanence magnetization in Fe/SiO2 increased notably with milling time, reaching 68.47 Oe and 8.73 emu g−1, respectively. The Fe/Fe2O3/SiO2 and FeSiO2 nanocomposites exhibited the maximum values of coercivity (47.07 Oe) and remanence magnetization (12.24 emu g−1). Remarkably, the Fe/SiO2 nanocomposite displayed the highest saturation magnetization, measuring an impressive 176.07 emu g−1 after 30 h of milling, while FeCu/SiO2 reached 165.64 emu g−1 after 20 h. Overall, our findings suggest the Fe/SiO2 nanocomposite as a promising high-frequency soft magnetic material.