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Optical tweezers can control the position and orientation of individual colloidal particles in solution. Such control is often desirable but challenging for single-particle spectroscopy and microscopy, especially at the nanoscale. Functional nanoparticles that are optically trapped and manipulated in a three-dimensional (3D) space can serve as freestanding nanoprobes, which provide unique prospects for sensing and mapping the surrounding environment of the nanoparticles and studying their interactions with biological systems. In this perspective, we will first describe the optical forces underlying the optical trapping and manipulation of microscopic particles, then review the combinations and applications of different spectroscopy and microscopy techniques with optical tweezers. Finally, we will discuss the challenges of performing spectroscopy and microscopy on single nanoparticles with optical tweezers, the possible routes to address these challenges, and the new opportunities that will arise.