High-entropy oxides (HEOs) are an emerging class of materials whose compositional complexity has garnered attention because of their tailorable chemistries and unique properties arising from extreme configurational entropy. Solid-state methods are often employed to synthesize HEOs, but such methods result in poor material properties for catalytic processes, leaving HEOs less studied for catalysis. Here we utilize different wet-synthesis strategies to produce porous HEOs and investigate their performance in heterogeneous CO₂ hydrogenation to methane. Specifically, HEOs were synthesized using hydrothermal, co-precipitation, and solvothermal methods, resulting in different morphologies like platelets or spheres. Of the tested materials, HEOs with 2-D platelets derived from hydrothermally-synthesized high-entropy layered double hydroxides had superior catalytic performance, especially in low-temperature regimes (<300 °C). K-edge XANES indicated that metallic sites (Ni⁰-Co⁰) were formed during the reaction, and these metallic sites are dispersed into the HEO matrix which is confirmed by STEM/elemental mapping. This facile synthesis approach allows for realized synergy between the metallic sites and the HEO support, leading to superior performance for CO₂ methanation compared to low-entropy counterparts. Finally, this study illustrates how HEOs offer new avenues of tailorability in terms of the interplay between support, active site and reaction temperatures for heterogeneous catalysis.