Interface engineering of heterostructures has emerged as a promising approach to enhance the catalytic activity of nonprecious electrocatalysts. Herein, a novel amorphous cobalt sulfide-crystalline nickel iron layered double hydroxide (a-CoS@NiFe-LDH) hybrid material is presented for application as an electrocatalyst for oxygen evolution reaction (OER). Benefitting from the well-matched energy level structures, the a-CoS@NiFe-LDH catalyst delivers a low overpotential of 221 ± 14 mV at an OER current density of 20 mA cm -2 and a small Tafel slope of 83.1 mV dec -1 , showing good OER properties. First-principle computations reveal that the electronic interaction between amorphous cobalt sulfide (a-CoS) and crystalline nickel iron layered double hydroxide (NiFe-LDH) components within a-CoS@NiFe-LDH promotes the adsorbate evolution mechanism and reduces the adsorption energies for oxygen intermediates, thereby enhancing the activity and stability for OER. This work opens up a new avenue to enhance the OER catalytic efficiency via the construction of amorphous-crystalline heterostructures.