Magnetic refrigeration is an emerging new technology for cooling and gas liquefaction. The proper selection of magnetic working materials plays a key role in any design of a magnetic refrigerator. Properly fabricated amorphous rare-earth-metal-based alloys may be promising candidates for magnetic refrigeration applications. Their advantages include tailorable composition, low eddy current and hysteresis losses, improved corrosion resistance, and large specific area. To optimize the composition, bulk magnetic properties of selected Re70M30−xTx (with Re = Gd, Dy, Er, Ho, Tb and M, T = Ni, Fe, Cu, Al) alloys have been investigated in the 5–350 K temperature and 0–7 T DC field range. Far above the magnetic transition, all investigated alloys display a Curie-Weiss behavior consistent with the effective atomic moment of the Re-atoms present. The composition dependence of the Weiss constant reveals that although influenced by the presence of transition metals, the ReRe exchange plays the main role in magnetic interactions. Gd-based alloys display a tendency to form multiple phases, which is supported by the presence of Fe and suppressed by the addition of Al. Single-phase amorphous Re70M30−xTx alloys are characterized by transition temperatures below 200 K, and in spite of their inherently broad transitions, they often display a magnetic entropy change superior or comparable to that of crystalline alloys with similar transition temperatures. Consequently, rare-earth-based amorphous alloys are promising candidates for magnetic refrigeration applications.