Underwater pollution incidents occur frequently, and obtaining accurate information about their exact location and real-time situation is helpful for promptly formulating plans to contain and mitigate the situation. Autonomously adjusting the position of sensors for optimal coverage and monitoring of regions of interest (e.g., oil spill zones, chemical contamination areas) in real time is a significant challenge. To this end, this article proposes a hunting-style underwater sensor deployment based on the level set method. This method uses a gateway-like role to calculate the boundary and other parameters of the interest region based on an energy function used for positioning sensors. Subsequently, the sensors use these parameters as the basis to complete their migration toward the boundary of the interest region. This sensor migration can gradually evolve into a hunting deployment for the interest region. This paper also proposes two novel performance evaluation metrics—structural similarity and network energy balance—to evaluate the comprehensive performance of the proposed hunting-style deployment of underwater sensors. Extensive simulation experiments demonstrate the effectiveness of the proposed method.