To improve the field-effect mobility of all-inkjet-printed organic thin film transistors (OTFTs), a composite material consisted of carbon nanoparticles (CNPs) and poly(3-hexylthiophene) (P3HT) was reported by using homemade inkjet-printing system. These all-inkjet-printed composite OTFTs represented superior characteristics compared to the all-inkjet-printed pristine P3HT OTFTs. To investigate the enhancement mechanism of the blended materials, the percolation model was established and experimentally verified to illustrate the enhancement of the electrical properties with different blending concentrations. In addition, experimental results of OTFT contact resistances showed that both contact resistance and channel resistance were halved. At the same time, X-ray diffraction measurements, Fourier transform infrared spectra, ultraviolet-visible light, and photoluminescence spectra were also accomplished to clarify the material blending effects. Therefore, this study demonstrates the potential and guideline of carbon-based nanocomposite materials in all-inkjet-printed organic electronics.