This invention discloses an MRI-PET cephalic molecular imaging coil and an MRI cephalic molecular imaging system including this MRI-PET cephalic molecular imaging coil the said MRI-PET cephalic molecular imaging coil is an integrated and nested structure, with a molecular signal acquisition assembly installed on the peripheral surface of the MRI cephalic RF coil, the said molecular signal acquisition assembly including a crystal gamma-ray detector and photoelectric conversion structure the said photoelectric conversion structure is semi-conductors, having an effect in preventing the impact of magnetic field on gamma-ray imaging, hence making it possible to obtain precision fusion images of magnetic resonance and molecular imagery and ensuring consistency of physiological and biochemical information in spatial location and temporal synchronization.