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This work demonstrates the capabilities and advantages of a novel sintering technique to fabricate bulk composition gradient materials. Pressure distribution calculations were used to compare several tooling geometries for use with current-activated, pressure-assisted densification or spark plasma sintering to densify a gradient along the long dimension of the specimen. The selected rectangular tooling design retains a low aspect ratio to ensure a uniform pressure distribution during consolidation by using a side loading configuration to form the gradient along the longest dimension. Composition gradients of NixCu1−x, MoxNb1−x, and MoNbTaWHfx (x from 0 to 1) were fabricated with the tooling. The microstructure, composition, and crystal structure were characterized along the gradient in the as-sintered condition and after annealing to partially homogenize the layers. The successful fabrication of a composition gradient in a difficult-to-process material like the refractory multi-principal element alloy system MoNbTaWHfx shows the utility of this approach for high-throughput screening of large material composition spaces.