It is generally agreed that fuel exhaust from vehicles is the largest contributor to air pollution. Here’s a link to an article that gives an overview of different types of air pollution and their causes: http://www.greenfootsteps.com/air-pollution-article.html
The greatest contributor to air pollution is the burning of fossil fuels. This includes vehicle emissions and power plants. The greatest contributor, though hard to say for sure, is likely emissions from driving cars.
It also depends on the region, whether there are more cars or industries. In big cities vehicles probably cause the bigger problem. However in small towns cars might not have such a big impact. Industries on the other hand often are located on the outskirts of cities thus have a smaller direct impact on a air quality.
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