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.