The growing industrial demand for customized, high-carbon tool steels that are adapted to additive manufacturing (AM) technologies has driven their development. Laser powder bed fusion (PBF-LB/M) has emerged as a key AM technique for producing near-net-shape, high-performance tools. In this process, a focused laser beam melts metal powder layer by layer to form a component, subjecting the feedstock to repeated rapid melting followed by solidification at high cooling rates. These conditions create non-uniform cooling, with heat primarily dissipating through already solidified material, resulting in a short-term heat treatment. This cycle results in the development of thermal residual stresses within the solidified part. Additionally, alloy-specific phase transformations, such as the austenite-to-martensite transition, can occur, and they pose further challenges in PBF-LB/M processing of high-carbon tool steels. Consequently, specialized steels are needed to withstand these extreme processing conditions while delivering superior properties to extend tool service life. To design such high-carbon steels, we propose an experimental alloy design method using centrifugal casting. This approach allows for a preliminary evaluation of the phases and mechanical properties in the PBF-LB/M state, using small material quantities and short processing time. This efficient material screening technique has enabled the development of a novel high-carbon Fe85Cr4Mo1V1W8C1 tool steel, which exhibits exceptional mechanical and wear properties as well as excellent processability via PBF-LB/M without the need for substrate plate heating. The high cooling rates in this process lead to the formation of a fine, hierarchical microstructure consisting of martensite, austenite, and special carbides, as revealed by scanning electron microscopy, electron backscatter diffraction, and transmission electron microscopy. These phases contribute to significantly enhanced compressive strength and abrasive wear resistance compared to conventional high-carbon tool steels. Comprehensive characterization has also provided insights into the underlying deformation and wear mechanisms. In conclusion, the proposed alloy design approach for PBF-LB/M led to the development of a novel tool steel with substantial potential for advanced tool design.