Catalysis has been a key way of improving the efficiency-to-cost ratio of chemical and electrochemical processes. There have been recent developments in catalyst materials that enable the development of novel and more sophisticated devices that, for example, can be used in applications, such as membranes, batteries or fuel cells. Since catalytic reactions occur on the surface, most catalyst materials are based on open porous structures, which facilitates the transport of fluids (gas or liquid) and chemical (or electrochemical) specific surface activity, thus determining the overall efficiency of the device. Noble metals are typically used for low temperature catalysis, whereas lower cost materials, such as nickel, are used for catalysis at elevated temperatures. 3D printing has the potential to produce a more sophisticated fit for purpose catalyst material. This article presents the development, fabrication and performance comparison of three thermoplastic composites where PLA (polylactic acid), PVB (polyvinyl butyral) or ABS (acrylonitrile butadiene styrene) were used as the matrix, and nickel particles were used as filler with various volume fractions, from 5 to 25 vol%. The polymer–metal composites were extruded in the form of filaments and then used for 3D FDM (Fused Deposition Modeling) printing. The 3D printed composites were heat treated to remove the polymer and sinter the nickel particles. 3D printed composites were also prepared using nickel foam as a substrate to increase the final porosity and mechanical strength of the material. The result of the study demonstrates the ability of the optimized filament materials to be used in the fabrication of high open porosity (over 60%) structures that could be used in high-temperature catalysis and/or electrocatalysis.