A multi-step heat treatment is proposed to optimize the lamellar structure of as-cast high Nb containing TiAl alloys. The β-segregation is removed effectively after the first two step heat treatment, a short-time holding within β single phase field then annealing in α+β phase field. During the third step heat treatment, a subsequent low-temperature aging, new γ lamellae precipitate by the means of isolated nucleation or twin-related nucleation. After the proposed multi-step heat treatment, the alloy presents nano-scaled lamellar structure with the colony size about 140 μm.