One of the most significant and uncertain aspects of climate change projections is the impact of aerosols on the climate system. Aerosols influence the climate indirectly by interacting with nearby clouds leading to small changes in cloud cover, thickness, and altitude, which significantly affect Earth's radiative balance. Advancements have been made in recent years on understanding the complex processes and atmospheric interactions involved when aerosols interact with surrounding clouds, but further progress has been hindered by limited observations. The National Academies of Sciences, Engineering, and Medicine organized a workshop to discuss the usefulness of the classified observing systems in advancing understanding of cloud and aerosol interactions. Because these systems were not developed with weather and climate modeling as a primary mission objective, many participants said it is necessary for scientists to find creative ways to utilize the data. The data from these systems have the potential to be useful in advancing understanding of cloud and aerosol interactions. This publication summarizes the presentations and discussions from the workshop.