Aerosol forcing uncertainty represents the largest climate forcing uncertainty overall. Its magnitude has remained virtually undiminished over the past 20 years despite considerable advances in understanding most of the key contributing elements. Recent work has produced modest increases only in the confidence of the uncertainty estimate itself. This review summarizes the contributions toward reducing the uncertainty in the aerosol forcing of climate made by satellite observations, measurements taken within the atmosphere, as well as modeling and data assimilation. We adopt a more measurement-oriented perspective than most reviews of the subject in assessing the strengths and limitations of each; gaps and possible ways to fill them are considered. Currently planned programs supporting advanced, global-scale satellite and surface-based aerosol, cloud, and precursor gas observations, climate modeling, and intensive field campaigns aimed at characterizing the underlying physical and chemical processes involved, are all essential. But in addition, new efforts are needed: (a) to obtain systematic aircraft in situ measurements capturing the multi-variate probability distribution functions of particle optical, microphysical, and chemical properties (and associated uncertainty estimates), as well as co-variability with meteorology, for the major aerosol airmass types; (b) to conceive, develop, and implement a suborbital (aircraft plus surface-based) program aimed at systematically quantifying the cloud-scale microphysics, cloud optical properties, and cloud-related vertical velocities associated with aerosol-cloud interactions; and (c) to focus much more research on integrating the unique contributions of satellite observations, suborbital measurements, and modeling, to reduce the persistent uncertainty in aerosol climate forcing. Plain Language Summary Aerosols, such as airborne wildfire smoke, desert dust, volcanic and pollution particles, affect Earth's climate by reflecting (some also absorb) sunlight. These aerosol particles also play key roles in cloud formation and evolution, further affecting the planet's energy balance. The magnitudes of these effects, and even the underlying mechanisms, represent the largest uncertainty in climate modeling. Despite two decades of advances in many aspects of aerosol-climate science, aerosol climate forcing uncertainty is virtually undiminished. Yet, reducing this uncertainty is critical for any effort to attribute, mitigate, or predict climate changes. We adopt a measurement-oriented perspective to assess the strengths and limitations of measurement and modeling programs, and conclude that current and planned efforts need to continue. However, in addition, new efforts are needed: (a) to obtain aircraft in situ measurements that capture systematically aerosol particle properties for the major aerosol airmass types, globally, (b) to conceive, develop, and implement an aircraft and surface-based program aimed at filling gaps in our understanding of the interactions between aerosol particles and clouds, along with (c) much more research focused on integrating