This work introduces the Reverse Steam Rising Process (RSRP), a novel dissolution method, for the preparation of highly homogeneous organo-nickel composites. This approach enables gradual material dissolution, resulting in improved material integration. We investigate two distinct synthetic pathways: a direct organic material–nickel composite and a surfactant-assisted variation. Our findings demonstrate that the inclusion of a surfactant significantly improves the properties of the resulting organo-nickel composite. The RSRP method differs from traditional synthesis methods in that it utilizes reverse steam condensation to create a highly porous, multi-level structure. This unique structure significantly boosts the material’s electrocatalytic performance, particularly for the oxygen evolution reaction (OER). The Ni-MOF-CTAB catalyst exhibits an overpotential of 397 mV at 10 mA cm⁻² and a Tafel slope of 183 mV dec⁻¹, outperforming pristine Ni-MOF. The hierarchical design promotes superior ion and gas transport, while the distinctive organometallic configuration optimizes electronic interactions critical for OER activity. This innovative process enables precise control over both the micro- and nanoscale morphology of the nickel-based catalyst, ultimately leading to superior performance metrics. This advancement offers a new pathway for developing high-performance nickel organometallic materials for diverse electrocatalytic applications.