Designing highly-efficient and pH-universal electrocatalysts for overall water-splitting reactions is important for the sustainable production of hydrogen. Herein, NiRu nanoparticles encapsulated into N-doped carbon (NiRu@NC) are fabricated with the assistance of MOF for hydrogen evolution reaction (HER) and also evolved into core–shell structured nanomaterials with abundant interfaces for oxygen evolution reaction (OER, Ni/RuOx@C). Benefiting from optimized electronic structure, interfacial synergy effect and special core–shell structure (~150 nm), the newly developed electrocatalysts present remarkable electrocatalytic activities with small overpotentials to drive 10 mA cm−2 for the HER (19 mV in alkaline, 80 mV in neutral, 20 mV in acid) and OER (252 mV, 316 mV, 211 mV). Moreover, the obtained electrocatalysts exhibit outstanding catalytic performances for overall water-splitting in a two-electrode system with 1.53 V and 1.67 V to drive 10 mA cm−2 in basic and neutral electrolyte, respectively. Remarkably, a small potential of 1.47 V is required to deliver 10 mA cm−2 in acidic media and no significant decay of the activity is observed. This work paves the way for designing a novel class of electrocatalyst that can not only exhibit remarkable electrocatalytic water splitting performances in various conditions, but also possess excellent stabilities for future generation of clean energy.