This study reports a characterization of the real part of dry particle refractive index (n) at 532 nm based on airborne measurements over the United States, Canada, the Pacific Ocean, and the Gulf of Mexico from the 2012 Deep Convective Clouds and Chemistry (DC3) and 2013 Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) campaigns. Effective n values are reported, with the limitations and uncertainties discussed. Eight air mass types were identified based on criteria related to gas-phase tracer concentrations, location, and altitude. Average values of n for these air types ranged from 1.50 to 1.53. Values of n for the organic aerosol (OA) fraction (nOA) were calculated using a linear mixing rule for each air mass type, with 1.52 shown to be a good approximation for all OA. Case studies detailing vertical structure revealed that n and nOA increased with altitude, simultaneous with enhancements in the mass fraction of OA. Values of nOA were positively (negatively) correlated with the O:C (H:C) ratio in the absence of biomass burning influence; in contrast, the cumulative data set revealed a slight decrease in nOA as a function of the O:C ratio. The performance of parametric (multiple linear regression) and nonparametric (Gaussian process regression) methods in predicting n based on aerosol composition data is discussed. It is shown that even small perturbations in n values significantly impact aerosol optical depth retrievals, radiative forcing, and optical sizing instruments, emphasizing the importance of further improving the understanding of this important aerosol property.