Herein, the strategy of homogenous inclusion of nanoparticles within the surface and interlayers of 2D MXenes is established to achieve effective oxygen evolution reaction (OER) performance. A greater quantity of nano‐sized Ni(OH)₂ particles is uniformly anchored on multilayered accordion‐like nanosheets of Ti₃C₂T_x. The strong interconnection of Ni(OH)₂ on Ti₃C₂T_x promotes synergistic effects and improves electron transfer properties alongside the intrinsic OER activity. The Ti₃C₂T_x‐Ni(OH)₂‐4 demonstrates remarkable OER activity by exhibiting a lower overpotential (235.54 mV at 10 mA cm⁻²) in alkaline conditions. Increased electrochemical active surface area (2.925 mF cm⁻²), lower charge transfer resistance, lowering the reaction barrier, and stabilizing/converting essential intermediates via the Ti₃C₂T_x‐Ni(OH)₂ electrocatalyst synergistically improve OER activity. The effective interaction between Ti₃C₂T_x and Ni(OH)₂ in Ti₃C₂T_x‐Ni(OH)₂ improves stability during long‐term operations. Moreover, a Ti₃C₂T_x‐Ni(OH)₂‐4||Pt/C cell has 1.7V at 10 mA cm⁻¹ . It can be deduced that the usage of Ni(OH)₂ as an electrocatalyst together with Ti₃C₂T_x can provide noteworthy water‐splitting properties.