Magnetic resonance imaging (MRI) is an inherently insensitive imaging modality, due to low thermal spin polarization at typical clinical magnetic field strength and room temperature. Dynamic nuclear polarization (DNP) has the potential to increase the magnetic resonance signal of the underlying material by 3–4 orders of magnitude through enhanced nuclear spin alignment. In this chapter, we describe the application of the DNP technique to silicon particles and nanoparticles for background-free real-time molecular MR imaging.