Biodegradable metallic glasses are used as disposable green devices whose constituents decompose into harmless byproducts, leaving no residual waste and requiring no removal surgery. Here, the large size Ca-based (Ca65Mg15Zn20) bulk metallic glasses (BMGs) were fabricated by consolidating gas-atomized metallic glassy alloy powder using a spark plasma sintering (SPS) technique. The effects of sintering temperature on structure, mechanical properties, and biodegradation rate of the developed Ca-based BMGs in Hank's solution were evaluated. The high-strength consolidated samples with a fully glassy phase and suitable biodegradation rate were produced by the SPS process at a sintering temperature of 120 °C with a loading pressure of 600 MPa. The Ca–Mg–Zn bulk metallic glass alloys developed by the SPS process can offer excellent properties and satisfy large sample-size requirements, which opens possibilities of application as biodegradable materials.