The effects of Fe2B-grain orientation on microstructure and properties of bulk Fe2B intermetallic fabricated by directional and ordinary solidification techniques have been investigated. The results show that unidirectional solidified Fe2B intermetallic possesses a strong (002) texture in the transverse direction owing to the opposite unidirectional heat-squeeze effect while random Fe2B grains can be produced under ordinary solidification conditions. The nonoriented Fe2B intermetallic has the highest linear expansion coefficient of 13.04 × 10−6 °C−1 while the microhardness and fracture toughness of transverse Fe2B intermetallic in the (002) plane are larger than those of Fe2B with other grain orientations and their values are ∼18.72 GPa and 6.42 MPa·m1/2, respectively. Liquid zinc corrosion results indicate that unidirectional Fe2B intermetallic with long axis perpendicular to the direction of liquid zinc corrosion displays the best corrosion resistance to liquid zinc owing to its beneficial barrier effect. The FeB transition phase can naturally form and grow parabolically during liquid zinc corrosion.