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A facile preparation of bio-inspired and morphology controllable catalytic electrode FeS@MoS₂/CFC, featuring a carbon fiber cloth (CFC) covered with FeS dotted MoS₂ nanosheets, has been established. Synergy between the CFC as a self-standing conductive substrate and the FeS nanoparticle dotted MoS₂ nanosheets with abundant active sites makes the noble-metal-free catalytic electrode FeS@MoS₂/CFC highly efficient in nitrogen reduction reaction (NRR), with an ammonia production rate of 8.45 μg h⁻¹ cm⁻² and excellent long-term stability at −0.5 V in pH neutral electrolyte. Further electrolysis in acidic and alkaline electrolytes revealed the overall NRR catalytic activity of this electrode over a wide pH range.