A comparative study of electron-beam and pulsed-laser irradiation effects in metallic glasses has been performed in order to understand the relationship between magnetic behavior and select variations in the structural characteristics of alloy phases. Samples of ${\mathrm{Fe}}_{81}$${\mathrm{B}}_{13.5}$${\mathrm{Si}}_{3.5}$${\mathrm{C}}_{2}$ metallic glass were irradiated with a pulsed excimer laser (\ensuremath{\lambda}=308 nm, \ensuremath{\tau}=10 ns), with a high-energy electron beam (W=7 MeV), and with low-energy electron beams (W=30 and 50 keV). Irradiation-driven changes in the magnetic anisotropy and phase equilibrium of alloy samples were studied by M\"ossbauer spectroscopy and scanning electron microscopy. Complementary information was obtained using energy-dispersive x-ray analysis. High-energy electron-beam irradiation was found to induce an out-of-plane magnetic anisotropy due to changes in the chemical short-range order. Low-energy electron-beam irradiation resulted in the formation of crystalline regions, in which \ensuremath{\alpha}-Fe, Fe-Si, ${\mathrm{Fe}}_{3}$B, ${\mathrm{Fe}}_{2}$B, and clusters of \ensuremath{\gamma}-Fe were identified. Interpretation of these results is given in terms of radiation-enhanced diffusion. Pulsed-excimer-laser irradiation was found to induce controlled magnetic anisotropy without onset of bulk crystallization in the ${\mathrm{Fe}}_{81}$${\mathrm{B}}_{13.5}$${\mathrm{Si}}_{3.5}$${\mathrm{C}}_{2}$ amorphous system. The effect of excimer-laser-induced amorphization was evidenced in thermally annealed ${\mathrm{Fe}}_{81}$${\mathrm{B}}_{13.5}$${\mathrm{Si}}_{3.5}$${\mathrm{C}}_{2}$ samples and explained using melt model calculations. In all cases studied, the key to explaining the irradiation-induced property modifications is the underlying alloy microstructure.