The El Niño-Southern Oscillation (ENSO) stands out as the most significant tropical phenomenon in terms of climatic magnitude resulting from ocean–atmosphere interaction. Due to its atmospheric teleconnection mechanism, ENSO influences various environmental variables across distinct atmospheric scales, potentially impacting the spatiotemporal distribution of atmospheric aerosols. Within this context, this study aims to evaluate the relationship between ENSO and atmospheric aerosols across the entire Legal Amazon during the period from 2006 to 2011. Over this five-year span, four ENSO events were identified. Concurrently, an analysis of the spatiotemporal variability of aerosol optical depth (AOD) and Black Carbon radiation extinction (EAOD-BC) was conducted alongside these ENSO events, utilizing data derived from the Aerosol Robotic Network (AERONET), MERRA-2 model, and ERSSTV5. Employing the Windowed Cross-Correlation (WCC) approach, statistically significant phase lags of up to 4 to 6 months between ENSO indicators and atmospheric aerosols were observed. There was an approximate 100% increase in AOD immediately after El Niño periods, particularly during intervals encompassing the La Niña phase. The analysis of specific humidity anomaly (QA) revealed that, contrary to expectations, positive values were observed throughout most of the El Niño period. This result suggests that while there is a suppression of precipitation events during El Niño due to the subsidence of drier air masses in the Amazon, the region still exhibits positive specific humidity (Q) conditions. The interaction between aerosols and humidity is intricate. However, Q can exert influence over the microphysical and optical properties of aerosols, in addition to affecting their chemical composition and aerosol load. This influence primarily occurs through water absorption, leading to substantial alterations in radiation scattering characteristics, and thus affecting the extinction of solar radiation.