is developed by Fritz Haber and Carl Bosch. [3] The process converts nitrogen (N 2 ) to ammonia (NH 3 ) by a reaction, also called nitrogen reduction reaction (NRR), with hydrogen (H 2 ) using a metal catalyst under high temperatures and pressures. The worldwide NH 3 production is about 140 million tonnes year −1 . [4] Unfortunately, Haber method has become one of the largest industrial energy consuming sources. Meanwhile, 1 ton of NH 3 is produced accompanied with 2 tonnes of CO 2 emissions. Currently, more than 1.6% of global CO 2 is emitted while ammonia is generated. [4] In addition, H 2 production and N 2 purification are also considered as energy intensive processes. Therefore, an environmentally friendly alternative synthesis process with no CO 2 emissions and low energy demand is desired.The electrochemical method assisted by earth-abundant materials has been utilized widely for the chemical energy conversion. [5] Earth-abundant metal compound catalysts, such as MoS 2 , [6] NiS 2 , [7] CoS 2 , [8] FeS 2 , [9] CoSe 2 , [10] CoP, [11] and MoP, [12] have been developed and exhibited good electrocatalytic activity for hydrogen evolution reaction (HER). Besides, MoS 2 , [13] SnS 2 , [14] carbon materials, [15] copper oxide, [16] etc., demonstrated CO 2 reduction reaction (CO 2 RR) by using electrolysis method. The Faradaic efficiency (FE) for HER and CO 2 RR electrolyzed by earth-abundant electrocatalysts can be achieved 99 and 90%, respectively. [9,17] However, the electrochemical synthesis of ammonia is still few. Therefore, the utilization of earth-abundant materials as efficient NRR active catalysts is of paramount importance. One report indicated that the maximum theoretical energy efficiency for the electrochemical reaction was estimated to be ≈45.9% if hydrogen evolution would be completely suppressed. [18] To date, however, it is still a challenge to convert N 2 and H 2 catalytically to NH 3 due to high activation energy of NN bond cleavage to form N 3− on the surface of catalysts as a rate-limiting step. [19] The ammonia synthesis through electrolytical method is still in its infancy. Most researches on electrochemical production of ammonia were based on molten salt electrolytes at high temperature and pressure. [20] Also, other researches indicated that the liquid solution, such as organic solvents, [21] ionic liquids, [22] and aqueous electrolyte [23] could be used as electrolytes for N 2 electrolysis with transition metal complexes as the electrocatalysts. Although aqueous electrolyteThe generation of ammonia, hydrogen production, and nitrogen purification are considered as energy intensive processes accompanied with large amounts of CO 2 emission. An electrochemical method assisted by photoenergy is widely utilized for the chemical energy conversion. In this work, earth-abundant iron pyrite (FeS 2 ) nanocrystals grown on carbon fiber paper (FeS 2 /CFP) are found to be an electrochemical and photoactive catalyst for nitrogen reduction reaction under ambient temperature and pressure. The electroche...