This research has been focused on the intricacies of Ti-5553 alloy, a promising material for aerospace applications, employing the laser powder bed fusion (LPBF) process. The assessment of printability through the LPBF approach was carried out. The effects of volumetric energy density (VED) on the resulting microstructure and mechanical properties were investigated. An optimal VED was identified that results in a remarkable relative density, surface roughness, and uniform hardness distribution in as printed components. Moreover, the influence of α precipitate morphology on mechanical properties was a focal point of our investigations. By selecting extreme VEDs within an appropriate melting mode, comprehensive analyses using advanced electron microscopy, X-ray computed tomography, and mechanical tests were performed to evaluate the quality and microstructural development in the LPBF-made parts. The presence of intragranular nonlamellar α particles was identified as a key contributor to the balance between ductility and impact toughness. Furthermore, the conducted work introduced a novel approach—laser postexposure treatment during LPBF—to control microstructure formation, resulting in uniform and elongated grains, comparable with directionally solidified products used for enhanced creep resistance. Higher ultimate strength values were recorded for samples printed parallel to the building direction, primarily attributed to transgranular fracture. This finding offers valuable insights into the optimization of build orientations for enhanced mechanical performance. Additionally, the challenges posed by rapid heating and solidification rates through postprocessing heat treatment were addressed. Tailored in situ and ex situ heat treatment cycles were shown to effectively modify microstructure and enhance mechanical properties.