Abstract-In the attempt to develop a clean process, study has been conducted to determine the effect of absorbed CO 2 gas as source of carbon to the case hardening of treated mild steels in the recently developed process of electro-carburisation in non-toxic molten carbonate salts. The concentration of CO 2 in the process was varied by purging a CO 2 and N 2 mixture at flow rate ratios of CO 2 :N 2 of 200:0, 150:50, 100:100, 50:150 and 0:200 mL.min -1 . Electro-carburisation was performed in two types of molten salt electrolyte i.e. a mixed anion Na 2 CO 3 -NaCl (mole ratio 4:1) and a pure carbonate Li 2 CO 3 -K 2 CO 3 (1:1 mole ratio). A voltage of 2.5V was applied between mild steel cathode and an inert SnO 2 anode at a carburisation temperature of 800 o C for 60 minutes. The results show that greater CO 2 concentration produced samples with greater surface hardness and thicker case-hardening, attributed to the increased availability of the electro-active carbon source which was generated by absorption of CO 2 . Electro-carburisation in Li 2 CO 3 -K 2 CO 3 and Na 2 CO 3 -NaCl gave surface hardness of 1075 ± 25 HV, however Li 2 CO 3 -K 2 CO 3 (540 thickness) gave thicker case depth compared to Na 2 CO 3 -NaCl (500 thickness). This is thought to be due to the amount of carbon deposited in each salt; 12.70 wt.% C in Li 2 CO 3 -K 2 CO 3 and 11.10 wt.% C in Na 2 CO 3 -NaCl.Index Terms-Molten salt, carburisation, carbonate salt, surface hardness, case depth.