Nickel-iron/magnesium/aluminum　bimetallic　catalysts　were　prepared　by　the　calcination　and　reduction　of　nickel-magnesium-iron-aluminum　hydrotalcite-like　compounds.　Characterization　suggests　that,　at　iron/nickel≤0.5,　both　nickel　and　iron　species　are　homogeneously　distributed　in　the　hydrotalcite　precursor　and　incorporated　into　the　Mg(Ni,　Fe,　Al)O　periclase　after　calcination,　giving　rise　to　uniform　nickel-iron　alloy　nanoparticles　after　reduction.　Ni-Fe/Mg/Al　(Fe/Ni=0.25)　exhibits　the　best　catalytic　performance　for　the　steam　reforming　of　tar　derived　from　the　pyrolysis　of　biomass.　It　is　suggested　that　the　uniform　nickel-iron　alloy　nanoparticles　and　the　synergy　between　nickel　and　iron　are　responsible　for　the　high　catalytic　performance.　Moreover,　the　Ni-Fe/Mg/Al　catalyst　exhibits　much　better　regenerability　toward　oxidation-reduction　treatment　for　the　removal　of　deposited　coke　than　that　of　conventional　Ni-Fe/α-Al2O3.　This　property　can　be　attributed　to　the　better　regeneration　of　Ni-Fe　alloy　nanoparticles　through　the　formation　and　reduction　of　Mg(Ni,　Fe,　Al)O.　Copyright　©　2014　WILEY-VCH　Verlag　GmbH　&　Co.　KGaA,　Weinheim.