Rare earth-doped nickel (Ni-RE) alloys are very attractive for the neutron shielding application for excellent neutron absorption and good mechanical behavior. Ni-RE intermetallics are important for their precipitation reinforcement in Ni alloys. In this work, Ni-RE intermetallics have been founded to be Ni grain refiners, which has been proved both by nucleation crystallography analysis and experiments. Ni-RE intermetallics could work as heterogeneous nucleation well, either different in atomic structures (for example, Ni17RE2, Ni5RE, Ni7RE2, Ni3RE, Ni2RE having matching orientation relationships as (111)Ni // (0004)Ni17Gd2 with
[
1
1
¯
0
]
Ni
/
/
[
01
1
¯
0
]
Ni17Gd2
, (111)Ni // (0002)Ni5Gd with
[
1
1
¯
0
]
Ni
/
/
[
01
1
¯
0
]
Ni
5Gd
, (111)Ni // (00018)Ni7Gd2 with
[
1
1
¯
0
]
Ni
/
/
[
01
1
¯
0
]
Ni7Gd2
, (111)Ni // (00012)Ni3Gd with
[
1
1
¯
0
]
Ni
/
/
[
01
1
¯
0
]
Ni3Gd
, (111)Ni // (222)Ni2Gd with
[
1
1
¯
0
]
Ni
/
/
[
1
1
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0
]
Ni2Gd
) or different in rare earth element (for example, (111)Ni // (0002)Ni5RE with
[
1
1
¯
0
]
Ni
/
/
[
01
1
¯
0
]
Ni5RE
is general matching orientation relationships (ORs) of Ni5RE (RE = Sc, Y, La ~ Lu) for Ni grains). When RE dopant mass fraction is 1 wt%, the grain size is reduced from ~50 μm to 15 μm, and the refinement effect reaches the best. The work proposes Ni-RE intermetallics as good heterogeneous nuclei for Ni grains with an atomic level understanding and provides theoretical guidance for high-strength nickel alloy design.