Abstract: The present disclosure discloses a high zirconia brick and a preparation process and use thereof. The high zirconia brick includes the following components in percentage by weight: 40-99% of zirconia, 0.1-60% of alumina, and 0.1-40% of yttria, iron oxide, titania, magnesia, calcia, and silica in total. In the present disclosure, heating and annealing cooling are controlled by means of curved temperature control, and a high zirconia brick prepared has uniform and segregation-free distribution of all elements and consistent overall density, without defects such as needle-like pores, bubble retention, and surface cavities. The high zirconia brick prepared by the technological method has features of short delivery cycles of products and customizable production.