Ni-Fe/Al2O3　alloy　catalysts　obtained　from　Ni3-xFexAl　(x = 0-1.2)　hydrotalcite-like　compounds　are　tested　in　CH4　decomposition　at　600°C　to　produce　H2　and　carbon.　By　calcination　at　500°C,　nickel-iron-aluminum　hydrotalcite　is　decomposed　into　Ni(Fe,Al)O　solid　solution;　upon　reduction　at　800°C,　Ni-Fe　alloy　with　uniform　composition　and　the　average　size　of　9.4　to　10.3 nm　is　formed.　The　Ni-Fe/Al2O3　alloy　catalysts　exhibit　higher　catalytic　life　and　carbon　yield　than　the　Ni3Al　counterpart,　with　the　optimal　alloy　composition　being　Ni:　Fe = 4:1.　Carbon　nanotubes　are　produced　on　all　catalysts,　and　the　average　carbon　diameter　is　decreased　to　a　certain　degree　by　Ni-Fe　alloying.　XRD　indicates　that　Ni-Fe　alloy　is　less　sintered　than　Ni　metal　under　the　reaction　atmosphere,　which　may　account　for　the　decrease　in　the　carbon　diameter.　This　study　provides　a　way　for　the　preparation　of　a　uniform　Ni-Fe　alloy　catalyst　and　its　sintering　resistance　is　helpful　for　controlling　the　carbon　morphology.　©　2022　John　Wiley　&　Sons　Ltd.