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Creating nanosized pores in 2D materials can increase the edge sites, improve the mass transfer, and contribute to different physical properties, which shows potential applications in many fields including filtration membranes, electronics and energy storage devices, and catalysts. An iconic member of this type of material is porous graphene. Herein, a unique 2D layered double hydroxide (LDH) nanomesh is designed and synthesized as a new class of 2D holey materials. It represents the first case of exfoliation method for preparing 2D holey materials among all published reports. As an oxygen evolution reaction electrocatalyst, the 2D CoCo‐LDH nanomesh has apparently lower onset overpotential (220 mV) than that of compact nanosheets without holes (270 mV) owing to the pores through the plane that offer more highly active edge sites with lower coordination number and promote the mass diffusion. This work opens up a new avenue for designing 2D porous materials for energy conversion and storage. A unique two‐dimensional (2D) layered double hydroxide (LDH) nanomesh is synthesized as a new class of 2D holey materials. It represents the first case of exfoliation method for preparing 2D holey materials among all published reports. As an oxygen evolution reaction electrocatalyst, the nanomesh offers more active edge sites and promotes mass diffusion, owing to the pores through the plane. [ABSTRACT FROM AUTHOR]