Nitrogen containing graphene like structures were obtained by the pyrolysis of two pyrimidine polymers at 600 °C. Pyrimidine polymers were prepared by the base catalyzed aldol condensation reactions between 2-decyloxy-4,6-dimethylpyrimidine and two aromatic dialdehydes. Pyrolyzed products were shown to have a graphitic structure by Raman spectroscopy, scanning electron microscopy, and powder X-ray diffraction studies. The presence of nitrogen in the graphitic structures was proved by elemental analysis and energy dispersive X-ray analysis experiments. Fluorescence quenching experiments with poly(3-hexylthiophene) (P3HT) showed that the resultant graphitic material can act as an acceptor. These materials were tested in P3HT/graphene hybrid field effect transistors which exhibited higher mobilities and comparable on/off ratios compared to P3HT only devices.