The integration of laser direct energy deposition (L-DED) for manufacturing high-hardness D2 tool steel components presents a promising avenue for addressing the increasing complexity of product geometries demanded by modern industry. However, the inherent variability in microstructure and mechanical properties induced by L-DED across the build height necessitates the employment of post-processing techniques to achieve material homogeneity. This study explores the synergistic application of homogenization and deep cryogenic treatment (DCT) as a novel post-processing strategy aimed at mitigating microstructural inhomogeneities and enhancing the mechanical properties of L-DED-fabricated D2 tool steel. Initial analysis of the as-built samples revealed a microstructure characterized by a fine network of eutectic carbides enveloping an FCC matrix, which imposed constraints on martensite transformation during DCT. Homogenization was found to effectively alleviate these constraints, promoting compositional and microstructural uniformity and enabling a more consistent transformation to martensite across the samples upon subsequent DCT. The strategic combination of homogenization and DCT resulted in achieving uniformly distributed high hardness levels exceeding 750 HV throughout the entire sample, regardless of their initial positions within the build. This study demonstrates the potential of combining homogenization with DCT as an effective approach to enhance the structural integrity and mechanical performance of L-DED-fabricated D2 tool steel, offering valuable insights for the development of advanced manufacturing processes for alloyed materials.