Light‐absorbing atmospheric aerosols such as carbonaceous particles influence the climate through absorbing sunlight. The mixing states of these aerosol particles affect their optical properties. This study examines the changes in the mixing states and abundance of strongly light absorbing carbonaceous particles by using transmission electron microscopy (TEM) and single‐particle soot photometer (SP2), as well as of iron oxide particles, in Tokyo, Japan. TEM and SP2 use fundamentally different detection techniques for the same light‐absorbing particles. TEM allows characterization of the morphological, chemical, and structural features of individual particles, whereas SP2 optically measures the number, size, and mixing states of black carbon (BC). A comparison of the results obtained using these two techniques indicates that the peaks of high soot (nanosphere soot (ns‐soot)) concentration periods agree with those of the BC concentrations determined by SP2 and that the high Fe‐bearing particle fraction periods measured by TEM agree with that of high number concentrations of iron oxide particles measured using SP2 during the first half of the observation campaign. The results also show that the changes in the ns‐soot/BC mixing states primarily correlate with the air mass sources, wind speed, precipitation, and photochemical processes. Nano‐sized, aggregated, iron oxide particles mixed with other particles were commonly observed by using TEM during the high iron oxide particle periods. We conclude that although further quantitative comparison between TEM and SP2 data will be needed, the morphologically and optically defined ns‐soot and BC, respectively, are essentially the same substance and that their mixing states are generally consistent across the techniques. Key Points Occurrences of ns‐soot/BC from TEM and SP2 data are generally consistent across the techniques Abundance and mixing state of ns‐soot/BC fractions changed after rain and during weak wind period Aggregated‐Fe particles were found during high iron oxide particles concentration periods