High Nb-containing TiAl alloys have been deemed ideal candidates for demanding structural applications under high temperatures due to their appealing mechanical qualities and low density. Nonetheless, its inherent brittleness at room temperature remains a significant impediment to its processability. Herein, different concentrations of boron were added into the Ti45Al8Nb2Cr (Ti4582) alloy by vacuum arc melting to tailor the microstructure and corresponding mechanical properties. The coarse lamellar colonies were significantly refined via boron addition, while excessive boron addition did harm to the mechanical properties. The different morphologies of the borides (Bf or B27) profoundly influenced the microstructure and mechanical properties of as-prepared alloys. Further elemental distribution, phase constitution, lamellar colony size, and mechanical properties were systematically investigated. Noteworthily, trace boron additions effectively improved the mechanical properties of Ti4582-xB alloys with an optimal adjustment in Ti4582–0.2B, showing 673 MPa for room temperature ultimate tensile strength (UTS) with elongation of 1.3 % and 1623 MPa for ultimate compressive strength (UCS) with compressive strain of 32.5 %. The improved mechanical properties of Ti4582-xB were mainly attributed to grain refining and second phase strengthening. Moreover, the hindrance and accommodation for dislocations by deformed twins and reinforcements effectively enhanced the mechanical properties.