Intelligent wireless networks that comprise self-organizing autonomous vehicles equipped with punctual sensors and radio modules support many hostile and harsh environment monitoring systems. This work’s contribution shows the benefits of applying such networks to estimate clouds’ boundaries created by hazardous toxic substances heavier than air when accidentally released into the atmosphere. The paper addresses issues concerning sensing networks’ design, focussing on a computing scheme for online motion trajectory calculation and data exchange. A three-stage approach that incorporates three algorithms for sensing devices’ displacement calculation in a collaborative network according to the current task, namely exploration and gas cloud detection, boundary detection and estimation, and tracking the evolving cloud, is presented. A network connectivity-maintaining virtual force mobility model is used to calculate subsequent sensor positions, and multi-hop communication is used for data exchange. The main focus is on the efficient tracking of the cloud boundary. The proposed sensing scheme is sensitive to crucial mobility model parameters. The paper presents five procedures for calculating the optimal values of these parameters. In contrast to widely used techniques, the presented approach to gas cloud monitoring does not calculate sensors’ displacements based on exact values of gas concentration and concentration gradients. The sensor readings are reduced to two values: the gas concentration below or greater than the safe value. The utility and efficiency of the presented method were justified through extensive simulations, giving encouraging results. The test cases were carried out on several scenarios with regular and irregular shapes of clouds generated using a widely used box model that describes the heavy gas dispersion in the atmospheric air. The simulation results demonstrate that using only a rough measurement indicating that the threshold concentration value was exceeded can detect and efficiently track a gas cloud boundary. This makes the sensing system less sensitive to the quality of the gas concentration measurement. Thus, it can be easily used to detect real phenomena. Significant results are recommendations on selecting procedures for computing mobility model parameters while tracking clouds with different shapes and determining optimal values of these parameters in convex and nonconvex cloud boundaries.