Metal-organic frameworks (MOFs) are promising catalysts for producing clean energy and environmental-based applications. This paper reported one-pot encapsulation of guest molecules, e.g., thiourea (TU) and D-Glucose-6-phosphate disodium salt dihydrate (G6P-Na₂), into zeolitic imidazolate frameworks (ZIF-67), denoted as S@ZIF-67 and P@ZIF-67, respectively. The organic guest molecules offered the synthesis of cobalt-based materials (e.g., Co₃O₄, CoP, and CoS), embedded heteroatoms (P, N, and S) via carbonization. The materials were tested for hydrogen generation via sodium borohydride (NaBH₄) hydrolysis. ZIF-67, S@ZIF-67, and P@ZIF-67 displayed maximum hydrogen generation rates (HGR_max) of 27,273, 24,000, and 60,000 mL_H2 g_cat⁻¹ min⁻¹, respectively, using 20 mg of the catalyst and 0.2 wt.% of NaBH₄ at 60 °C. The materials were also investigated as potential catalysts for the adsorption and catalytic degradation of water pollutants such as organic dyes, e.g., methyl orange (MO) and Congo red (CR), with degradation efficiency of 100% and 99% in a short time (30–60 min).