We present the new promising method to improve the ductility of intermetallic compound, Ni3Al. Stoichiometric and Alrich Ni3A1 were unidirectionally grown at the growth rate of 24 mm/h by a floating zone method (FZ-UDS). The stoichiometric Ni3Al had a columnar-grained and single phase structure, whereas the Al-rich Ni3Al had a Ni3Al matrix with martensite-like precipitates. These alloys exhibited a large tensile elongation along the growth direction at room temperature. Fracture mode is a complete transgranular fracture in the stoichiometric Ni 3Al alloy, and a mixture of transgranular fracture of the matrix and cleavage of the martensite-like precipitates with cracking at the phase boundary in the Al-rich Ni3Al alloys.