From 1950 to 2015, more than 4.9 billion metric tons of new plastic materials were put into landfills or the environment. Unfortunately, this number will continue to increase due to the yearly production of over 350 million metric tons of plastic, of which 79% is quickly discarded. This plastic waste is not only a significant environmental issue but also a concern for human health. However, these wastes contain valuable amounts of energy and carbon that could be used as feedstock in the chemical industry. To combat the plastic waste crisis, there are ongoing efforts to transform these wastes into high-value chemicals through chemical upcycling. Our research has shown that earth-abundant zirconia nanoparticles can cleave the C-C bond in polyethylene to create a narrow distribution of small hydrocarbon molecules catalytically.[1] This material consists of nanoparticles of zirconia embedded in the walls of mesoporous silica, named as L-ZrO₂@mSiO₂. The mSiO₂ coating on zirconia nanoparticles helps to stabilize the coordinatively unsaturated surface sites needed for catalysis. Our DFT calculations show that these oxides can mediate C-C bond hydrogenolysis with activity comparable to Pt/C. This is due to L-ZrO₂@mSiO₂ containing a combination of small crystalline ZrO₂ with mSiO₂, which we hypothesize to contain a large number of ZrO_x defect sites that exhibit catalytic activity. A new bifunctional (hydroxy)organozirconium oxide species has been suggested for catalytic chemistry. The hydrogenolysis with L-ZrO₂@mSiO₂ is a previously unrecognized heterogeneous analog of the SOMC-catalyzed C-C cleavage processes.[2-4]