The dry reforming of methane (DRM) has been proposed as an efficient way to convert two greenhouse gases, namely CO2 and CH4 to syngas. However, most catalysts reported in the literature suffer from strong deactivation during the reforming reaction. The deactivation is caused by strong sintering of catalytically active nanoparticles and the formation of filamentous carbon. Herein a new synthesis procedure based on molecular layer deposition (MLD) is established to stabilize DRM catalysts under reaction conditions. Deactivation of a Ni/SiO2 reference catalyst was prevented by forming a defined porous net-like over-layer, which prevents the sintering and detachment of Ni nanoparticles by filamentous carbon. The MLD approach was further compared to the formation of an overlayer by atomic layer deposition (ALD), demonstrating the advantages of MLD forming hybrid organic-inorganic alucone layers over classical alumina ALD.