Spectral aerosol optical depth (AOD) estimation from satellite-measured top of atmosphere (TOA) reflectances is challenging because of the complicated TOA-AOD relationship and a nexus of land surface and atmospheric state variations. This task is usually undertaken using a physical model to provide a first estimate of the TOA reflectances which are then optimized by comparison with the satellite data. Recently developed deep neural network (DNN) models provide a powerful tool to represent the complicated relationship statistically. This study presents a methodology based on DNN to estimate AOD using Himawari-8 Advanced Himawari Imager (AHI) TOA observations. A year (2017) of AHI TOA observations over the Himawari-8 full disk collocated in space and time with Aerosol Robotic Network (AERONET) AOD data were used to derive a total of 14,154 training and validation samples. The TOA reflectance in all six AHI solar bands, three TOA reflectance ratios derived based on the dark-target assumptions, sun-sensor geometry, and auxiliary data are used as predictors to estimate AOD at 500 nm. The DNN AOD is validated by separating training and validation samples using random k-fold cross-validation and using AERONET site-specific leave-one-station-out validation, and is compared with a random forest regression estimator and Japan Meteorological Agency (JMA) AOD. The DNN AOD shows high accuracy: (1) RMSE = 0.094, R2 = 0.915 for k-fold cross-validation, and (2) RMSE = 0.172, R2 = 0.730 for leave-one-station-out validation. The k-fold cross-validation overestimates the DNN accuracy as the training and validation samples may come from the same AHI pixel location. The leave-one-station-out validation reflects the accuracy for large-area applications where there are no training samples for the pixel location to be estimated. The DNN AOD has better accuracy than the random forest AOD and JMA AOD. In addition, the contribution of the dark-target derived TOA ratio predictors is examined and confirmed, and the sensitivity to the DNN structure is discussed.