A few-layer graphene-based hybrid material with high thermal and chemical stability and reproducible and tunable electronic properties was fabricated by intercalation of N-methylpyrrolidone into a few-layer graphene combined with heat treatment. Depending on the process temperature, the obtained material could be produced with the following properties: a broad range of resistivity values (six to seven orders of magnitude) in combination with a high carrier mobility, a tunable band-gap (from 0 up to 3-4 eV) and sp² or sp³ hybridization of carbon atoms. The extremely strong step-like temperature dependence (within 10 °C) of its properties observed in the vicinity of two temperatures, 90 and 200 °C, seems to be important for various applications. The hybrid material opens viable routes to progress in the design of three-dimensional nanostructures.