The absence of slip systems makes amorphous structure very sensitive to the type of loading and extremely brittleness in tension. In the present work, The microstructure and mechanical properties of Zr-based alloys prepared by vacuum suction-cast in high content of O were investigated. The results show that the Zr-based alloy with gradient amorphous structure, has the extraordinary strength and ductility, with a maximum compressive strength of 1811.7 MPa and a plastic strain of 23.6%. The improvement of strength is due to the amorphous layer at the edge and the existence of nanoscaled amorphous particles and nanoscaled oxides at grain boundaries. Toughness phases such as CuZr in the centre store the dislocations to achieve the ductile deformation, resulting in the toughness enhancement of such alloy with a gradient structure.