Air pollution is one of the prime adverse environmental outcomes of urbanization and industrialization. The first step toward air pollution mitigation is monitoring and identifying its source(s). The deployment of a sensor array always involves a tradeoff between cost and performance. The performance of the network heavily depends on optimal deployment of the sensors. The latter is known as the location–allocation problem. Here, a new approach drawing on information theory is presented, in which air pollution levels at different locations are computed using a Lagrangian atmospheric dispersion model under various meteorological conditions. The sensors are then placed in those locations identified as the most informative. Specifically, entropy is used to quantify the locations’ informativity. This entropy method is compared to two commonly used heuristics for solving the location–allocation problem. In the first, sensors are randomly deployed; in the second, the sensors are placed according to maximal cumulative pollution levels (i.e., hot spots). Two simulated scenarios were evaluated: one containing point sources and buildings and the other containing line sources (i.e., roads). The entropy method resulted in superior sensor deployment in terms of source apportionment and dense pollution field reconstruction from the sparse sensors’ network measurements.