3D architecratured transition metal dichalcogenides constructed by atomically thin layers are appealing building blocks in various applications, such as catalysts, energy storage, conversions, sensors, and so on. However, the direct growth of 3D transition metal dichalcogenides architectures with high crystal quality and well‐controlled size/thickness remains a huge challenge. Herein, we report a facile, highly‐repeatable, and versatile chemical vapor deposition strategy, for the mass production of high‐quality 3D‐architecratured transition metal dichalcogenides (e.g., MoS2, WS2, and ReS2) and their alloys (e.g., WxMo(1–x)S2 and RexMo(1–x)S2) nanosheets on naturally abundant and low‐cost diatomite templates. Particularly, the purified transition metal dichalcogenides products exhibit unique and designable 3D biomorphic hierarchical microstructures, controllable layer thicknesses, tailorable chemical compositions, and good crystallinities. The weak interlayer interactions endow them with good dispersity in solutions to form stable additive‐free inks for solution‐processing‐based applications, for example, high‐permeable and high‐stable separation membranes for water purification, and efficient electrocatalysts for hydrogen evolution reactions. This work paves ways for the low‐cost, mass production of versatile transition metal dichalcogenides powder‐like materials with designable structures and properties, toward energy/environmental‐related applications and beyond.