Layered inorganic material, with large‐area interlayer surface and interface, provide an essential material platform for constructing new configuration of functional materials. Herein, we demonstrate a layered materials pillared with nanoclusters realizing high temperature thermal insulation performance for the first time. Specifically, systematic synchrotron radiation spectroscopy and finite element calculation analysis show that ZrOx nanoclusters served as “pillars” to effectively produce porous structures with enough boundary defect while maintaining the layered structure, thereby significantly reducing solid state thermal conductivity (∼0.32 W m−1·K−1, 298–573 K). Moreover, the layered inorganic silicate material assembled aerogel also exhibits superior thermal insulation performance from room temperature (0.034 W m−1·K−1, 298 K, air conditions) to high temperature (0.187 W m−1·K−1, 1073 K, air conditions) and largely enhanced compressive strength (42 kPa at 80% compression), which is the best layered material based aerogel that has achieved synergistic improvement in thermal and mechanical performance so far. Layered inorganic silicate aerogel pillared by nanoclusters will pave a new avenue for design of advanced thermal insulation materials under extreme conditions.This article is protected by copyright. All rights reserved