To overcome the issue of the sluggish kinetics in the oxygen evolution reaction (OER), the development of an efficient OER electrocatalyst with high intrinsic activity is very desirable for green hydrogen energy utilization from electrochemical water splitting. Herein, a facile and feasible solvothermal reaction of Sb, Se, DyCl3 and triethylenetetramine (teta) at 170 °C for 7 days achieved a new organic hybrid dysprosium selenidoantimonate [Dy(teta)2][SbSe4] (SbSe-1), which comprises discrete [SbSe4]3- and [Dy(teta)2]3+ ions. SbSe-1 was utilized in combination with acetylene black (AB), Ni nanoparticles and the porous Ni foam (NF) support to fabricate a Ni/SbSe-1@AB/NF electrode as an efficient anodic electrocatalyst, showing excellent OER electrocatalytic performance with a low overpotential of 269 mV at 10 mA cm-2. Although some antimony chalcogenides are used as electrocatalysts for the water splitting, organic hybrid lanthanide chalcogenidoantimonates applied as OER electrocatalysts have not emerged. Therefore, SbSe-1 offers the first example of an organic hybrid lanthanide chalcogenido-antimonate as an OER electrocatalyst.