We demonstrate that MoS₂ quantum dots (QDs) can be an effective and durable catalyst for the electrocatalytic N₂ reduction reaction (NRR), showing an NH₃ yield of 39.6 μg h⁻¹ mg⁻¹ with a faradaic efficiency of 12.9% at −0.3 V, far superior to MoS₂ nanosheets and outperforming most reported NRR catalysts. Density functional theory computations unravel that the MoS₂ QDs can dramatically facilitate N₂ adsorption and activation via side-on patterns, resulting in an energetically-favored enzymatic pathway with an ultra-low overpotential of 0.29 V.