The nickel-iron hydroxide-like catalyst for oxygen evolution reaction (OER) is prepared by an improved coprecipitation method. The crystallization degree of hydrotalcite-like compound is high, and the lamellar structure is homogeneous with no agglomeration, which helps to build efficient mass-transfer layer channel of OH ions. The NiFe layered double hydroxide (LDH)/carbon nanotubes (CNTs) electrode shows good performance and stability for OER. The potential of NiFe LDH/CNTs electrode is only 0.592 V (vs HgO/Hg) at 200 mA·cm−2 in 6 mol·L−1 potassium hydroxide (KOH) electrolyte, which shows excellent catalytic activity for OER. The NiFe LDH/CNTs electrode works continuously for 620 hours at 200 mA·cm−2, with the groove voltage only rises 0.1 V.