Holey 2D metal oxides have shown great promise as functional materials for energy storage and catalysts. Despite impressive performance, their processing is challenged by the requirement of templates plus capping agents or high temperatures; these materials also exhibit excessive thicknesses and low yields. The present work reports a metal‐based coordination polymer (MCP) strategy to synthesize polycrystalline, holey, metal oxide (MO) nanosheets with thicknesses as low as two‐unit cells. The process involves rapid exfoliation of bulk‐layered, MCPs (Ce‐, Ti‐, Zr‐based) into atomically thin MCPs at room temperature, followed by transformation into holey 2D MOs upon the removal of organic linkers in aqueous solution. Further, this work represents an extra step for decorating the holey nanosheets using precursors of transition metals to engineer their band alignments, establishing a route to optimize their photocatalysis. The work introduces a simple, high‐yield, room‐temperature, and template‐free approach to synthesize ultrathin holey nanosheets with high‐level functionalities.

The present work reports a simple and rapid disassembly/reassembly approach at room temperature to tailor functional metal oxides of 2D and 3D architectures.

Well-defined second-generation hot spots in end-to-end assembled gold nanobipyramids exhibit sufficient enhancement of the plasmonic field for single molecule detection.

Inspired by the design and performance of biological pores, polymer functionalization of nanopores has emerged as an evolving field to advance transport performance within the last few years.

The versatile qualities of gold coated magnetic nanoparticles for both optical and electrochemical detection, as well as the separation of analytes, make them an excellent choice for ultrasensitive biosensing applications.