The insulator Na₂Ta₄O₁₁ has been considered as a potential photocatalyst. However, little attention has been given to the synthesis of Na₂Ta₄O₁₁ nanoparticles, let alone the growth of two-dimensional (2D) layered Na₂Ta₄O₁₁ flake, which may bring innovative properties and promising applications. Here, the 2D thin-layer Na₂Ta₄O₁₁ flake was first produced by chemical vapor deposition (CVD) method, with the smallest thickness reported currently. We have also synthesized 2D Na₂Ta₄O₁₁ flake over 100 μm, which was the largest value over the 2D level reported to date. Our work proposed novel strategies to synthesize other 2D metal oxide material and endow the Na₂Ta₄O₁₁ more properties and applications.