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This article proposes a method of estimating the concentrations of particulate matter (PM2.5 and PM10) using public data, including road-traffic closed-circuit television (CCTV) images, Smart Seoul City data sensor environment information, and Korea Meteorological Administration data. The region-of-interest images and full scenes derived from CCTV footage were used as the basis for the deep learning model, which combines a convolutional neural network and long short-term memory, to establish the particulate matter (PM) concentration prediction methodology. In the experiment, the prediction accuracies corresponding to various types of mean values were calculated by training the model with various mean measurement values for the surface PM2.5 and PM10 concentrations, as well as the corresponding CCTV images and weather data at different time points. In the experiments performed under relatively stable PM concentrations, R2 generally exceeded 0.9 and tended to increase with an increasing range of mean concentration values. In particular, in sections with rapid changes in the PM concentration within an hourly interval, higher R2 values were obtained by the model trained with the average PM concentrations of the time series before and after image capture, outperforming the method that used prior mean observation values and better reflecting the current PM concentration.