Light absorption enhancement (Eabs) of black carbon (BC) aerosol following atmospheric aging is one of the most challenging issues in the assessment of aerosol radiative forcing. BC Eabs is constrained by complex particle morphologies; however, large uncertainties continue to occur due to certain morphological parameters, including primary particle size. The values of Eabs during BC aging is quantified with diverse primary particle sizes using the superposition T-matrix method (STM). The results show that the uncertainty of absorption enhancement due to the primary particle size of fully aged BC particles ranges from ~10% to 20%, while the uncertainties arising from varied BC volume-equivalent size and fractal dimension are ~20–30% and ~8–12%, respectively. The optical properties of BC particles with volume-equivalent radii ranging from 50 to 70 nm were largely influenced (up to ~50%) by inappropriate assumptions regarding primary particle size. The specific assumptions of primary particle size in optical modeling plays an important role in constraining BC Eabs.