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A hierarchical microstructure was obtained, including the unique interlaced dual-phase structure, the solidified molten pool, the coarse columnar B2 grains and fine equiaxed B19’ grains, and a great many nanoparticles, during laser powder bed fusion (LPBF) of NiTi alloys. The effect of laser processing parameter on the growth of nanoparticles was assessed. A combination of low laser power and high scanning speed was conducive to the formation of fine granular nanoparticles with a more uniform distribution. Subsequently, effects of rotation angle between adjacent layers on the compressive deformation behaviour of LPBF-processed NiTi alloys were studied. At a small rotation angle (6–36°), the samples could exhibit an excellent combination of high compressive fracture strength and ductility (e.g. 3094 MPa/39.85%). Meanwhile, samples with small rotation angle tended to get a large strain span for the martensite transformation stage and a large deformation capacity (e.g. 4.64% and 9.25% for θ = 6° and σmax = 800 MPa).