Recently, great effort has been applied to explore non-noble metal catalysts. However, the ambiguous understanding of active transfer mechanisms hinders the electrocatalysts design. [6][7][8] It has been reported that the appropriate design of the crystal distortion can improve catalytic performance for the modulated electronic structure of the active site. [9][10][11] Nevertheless, in the past, all the strategies focused on replacing the element of octahedron with others, which was inevitable for the change of intrinsic electronic structure caused by the introduction of other elements. [12,13] Meanwhile, most studies have focused on analyzing electronic structures while the contribution of structural changes for the generation of active phases is ignored chronically. [14][15][16] In fact, the active phase generated during the electrochemical process is considered to be the truly electrochemically active substance. [3,17,18] Besides, the coexistence of octahedral and tetrahedral in oxides such as spinel and chalcocite also limits further understanding of the accurate catalytic mechanism. [19,20] Notably, introducing strain not only generates the inner strain energy promoting the active phase transformation but also can tune the distortion degree of octahedral, thereby modulating their electronic structure and catalytic properties. [21] It is interesting to note that layered double hydroxides (LDHs) are composed entirely of octahedral. [22][23][24] Hence, the intrinsic effects of octahedral deformation can be well analyzed to help the development of advanced electrocatalysts. Moreover, it has excellent intrinsic activity comparable to precious metals, including RuO 2 and IrO 2 .Firstly, we use the density functional theory (DFT) calculations to reveal that tensile stress modifies the electronic structure. The distribution of e g and t 2g electrons was changed and the d band center was enhanced, optimizing adsorption energy and promoting OER process. Despite this, there remain many obstacles to introducing strain into the LDHs. As a kind of hydroxide, LDHs are very fragile and very easy to destroy in the process of producing internal stress. Dislocations have stress fields that are capable of generating the required tensile stress to modulate the catalytic performance and are able to modulate the catalytic performance (Figures S1 and S2, Supporting Information). Therefore, strain energy can be introduced by