Nanocarbon modified vermiculite porous ceramics with hydrophobicity were prepared using vermiculite as the starting materials and polyethylene terephthalate (PET) as the carbon precursor via the catalytic reaction method. The microstructures, hydrophobicity, and adsorption capacity of as-prepared porous ceramics were characterized by scanning electron microscope, water contact angle testing, and weight gaining, respectively. The results revealed that the nano-carbon generated from the pyrolysis of PET formed on the surface of the pores in ceramics. The water contact angle of as-prepared modified porous ceramics with 82% porosity was up to 123 °. The as-prepared porous ceramics showed highly efficient adsorption to oils and were very durable, and would be excellent candidate materials to separate the oil from the water/oil mixture.