This article reviews our recent results on the development of ferromagnetic bulk amorphous alloys prepared by casting processes. The multicomponent Fe-(Al,Ga)-(P,C,B,Si) alloys are amorphized in the bulk form with diameters up to 2 mm, and the temperature interval of the supercooled liquid region before crystallization is in the range of 50 to 67 K. These bulk amorphous alloys exhibit good soft magnetic properties, i.e., high Bs of 1.1 to 1.2 T, low Ho of 2 to 6 A/m, and high μe of about 7000 at 1 kHz. The Nd-Fe-Al and Pr-Fe-Al bulk amorphous alloys are also produced in the diameter range of up to 12 mm by the copper mold casting process and exhibit rather good hard magnetic properties, i.e., Br of about 0.1 T, high Ho of 300 to 400 kA/m, and rather high (JH)max of 13 to 20 kJ/m3. The crystallization causes the disappearance of the hard magnetic properties. Furthermore, the melt-spun Nd-Fe-Al and Pr-Fe-Al alloy ribbons exhibit soft-type magnetic properties. Consequently, the hard magnetic properties are concluded to be obtained only for the bulk amorphous alloys. The bulk Nd- and Pr-Fe-Al amorphous alloys have an extremely high Tx/Tm of about 0.90 and a small ΔTm(=Tm−Tx) of less than 100 K and, hence, their large glass-forming ability is due to the steep increase in viscosity in the supercooled liquid state. The high Tx/Tm enables the development of a fully relaxed, clustered amorphous structure including Nd-Nd and Nd-Fe atomic pairs. It is, therefore, presumed that the hard magnetic properties are due to the development of Nd-Nd and Nd-Fe atomic pairs with large random magnetic anisotropy. The Nd- and Pr-based bulk amorphous alloys can be regarded as a new type of clustered amorphous material, and the control of the clustered amorphous structure is expected to enable the appearance of novel functional properties which cannot be obtained for an ordinary amorphous structure.