Multimodal imaging-the ability to acquire images of an object through more than one imaging mode simultaneously-has opened additional perspectives in areas ranging from astronomy to medicine. In this paper, we report progress toward combining optical and magnetic resonance (MR) imaging in such a "dual" imaging mode. They are attractive in combination because they offer complementary advantages of resolution and speed, especially in the context of imaging in scattering environments. Our approach relies on a specific material platform, microdiamond particles hosting nitrogen vacancy (NV) defect centers that fluoresce brightly under optical excitation and simultaneously "hyperpolarize" lattice [Formula: see text] nuclei, making them bright under MR imaging. We highlight advantages of dual-mode optical and MR imaging in allowing background-free particle imaging and describe regimes in which either mode can enhance the other. Leveraging the fact that the two imaging modes proceed in Fourier-reciprocal domains (real and k-space), we propose a sampling protocol that accelerates image reconstruction in sparse-imaging scenarios. Our work suggests interesting possibilities for the simultaneous optical and low-field MR imaging of targeted diamond nanoparticles.