Aerosols can invigorate deep convective clouds (DCCs) directly by nucleating more cloud droplets, named as Primary Aerosol Convective Invigoration (PAI). However, the covarying Meteorology‐Aerosol Invigoration (MAI) effect on DCC has been a long‐standing issue in quantifying PAI's contribution. Here, observations show that PAI causes positive feedback from DCC to meteorology, further invigorating DCC through enhanced humidity, updraft and destabilization, thereby adding to MAI. Further, PAI is separated from MAI observationally by quantifying the sensitivity of DCC properties to aerosol changes under fixed meteorology through the artificial neural network. When fine aerosol changes from the cleanest to optimal concentration (5 μg m−3), PAI contributes 72% ± 2% of the total aerosol‐associated cloud top cooling by 12°C, 42% ± 4% of the 30% prolonged lifetime, and 50% ± 4% of the more than doubled rainfall. This result underlines the comparable magnitudes of PAI and MAI, which have not been considered until now in weather and climate prediction. Plain Language Summary: Aerosol has been observed and simulated to be directly associated with the development of strong convective storms, termed as Primary Aerosol Convective Invigoration (PAI). However, the current consensus is that meteorology also affects aerosol distribution, that is, there is covariability between meteorology and aerosols, possibly producing an overestimated observed association between aerosols and storms. Disentangling the PAI effect from the covarying meteorology‐aerosol effect on the storms has been a long‐standing challenge. Here, based on an artificial neural network technology, we quantify the PAI effect which explains ∼2/3 of the observed total aerosol‐driven variation in cloud top height, and 40%–50% of lifetime and rainfall when aerosol changes from the cleanest state to ∼5 μg m−3 concentration. Furthermore, we provide the first‐of‐its‐kind observational support for the Meteorology‐Feedback Aerosol Convective Invigoration (FAI). PAI modifies the environment and feeds back to the meteorology, which would become more conducive to storm development. This study demonstrates that fine aerosols have a large impact on the vigor of tropical deep convective clouds, which in turn adjusts environmental properties and meteorology. This is a manifestation of the way by which aerosol modulates tropical convection and, through that, further influences atmospheric circulation. Key Points: Total aerosol‐driven convective invigoration can be separated into primary and meteorology‐covarying aerosol effectsPrimary aerosol invigoration is observed to alter the environment to be more conducive for convection in a positive feedback loopPrimary invigoration explains ∼2/3 of the observed total aerosol‐driven variation in cloud top height and 40%–50% of lifetime and rainfall [ABSTRACT FROM AUTHOR]