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Three cobalt-based metal-organic framework (MOF)-derived catalysts were developed for photothermal hydrogen production via ammonia decomposition. The selected MOFs were from distinct families, featuring carboxylate and imidazole linkers, and diverse in terms of porosity. The resulting catalysts consisted of uniform and homogeneously dispersed cobalt nanoparticles embedded within a carbon matrix. The carboxylate-based MOF-74 derived catalyst showed the highest initial activity, but gradually deactivated. ZIF-67 derived catalyst, however, demonstrated stable performance. The synergy between photo and thermal effects was confirmed. Additionally, this catalyst was found to be also effective in ammonia synthesis, potentially closing the loop for sustainable ammonia utilization., (© 2024 Wiley‐VCH GmbH.)