The microstructure and materials performance of Laser Powder Bed Fusion-fabricated (LPBFed) NiTi shape memory alloys (SMAs) varies depending on the laser parameters and building directions. This study initially optimized the laser processing parameters (laser power and scanning speed) for LPBFed NiTi SMAs to enhance their printing quality and mechanical properties. We determined that with fixed hatch spacing of 80 μm and layer thickness of 30 μm, the laser power of 105 W, and scanning speed of 600 mm/s produced the best results. Subsequently, the corrosion behavior of LPBFed NiTi SMAs built in three different building directions (0°, 45°, 90°) was investigated in 0.9 wt.% NaCl solution at 37 °C. The electrochemical data revealed that the corrosion current density (Icorr) decreased with increasing building direction angle (Icorr-90° <Icorr-45° <Icorr-0°). The corrosion resistance followed the order of 0° sample ˂ 45° sample ˂ 90° sample. These findings were attributed to the difference in the grain size and boundary density. Higher boundary densities enhanced the electron activity capacity and the element diffusion rates, facilitating the rapid formation of a protective film and thus improving the corrosion resistance. This new insight into the anisotropy of corrosion behavior relative to building directions can inform the design of NiTi-SMA products and improve their reliability in tissue engineering applications.