Series of intensive investigations into porous, morphologically distinctive and well-defined zircons have been conducted. Single-to-multiple layered zircons were controllably synthesized for the first time by modulating parameters of hydrothermal duration, pH, and concentration under low-temperature hydrothermal conditions. The layered zircons possess high specific surface area and micro-to-meso pore structure, which make them suitable candidates for catalyst supports applied at high temperature. The larger d-spacing and the shift of the crystal plane (200) of these hydrothermal zircons are interpreted mainly for the structural incorporation of fluorine ions and OH groups.