Historically, domestic and wild animals have been used as sentinels for human exposure to environmental contaminants, providing an early warning system for public health intervention. Since domestic animals, particularly cats and dogs, share their (indoor) environment with humans, they can respond to or be affected by toxic assaults like their owners. Given that, the potential for pets to act as biosentinels of human exposure to environmental contaminants has been explored in many scientific papers. In this chapter, an overview of literature studies of how pets have served as sentinels for human health effects resulting from exposure to several classes of environmental contaminants (such as metals, persistent organic pollutants, flame retardants, and polycyclic aromatic hydrocarbons) is reported and discussed. The possible links among the studies and/or the potential gaps in knowledge and research were also investigated. The presented studies indicated that cats and dogs are exposed to complex mixtures of industrial chemicals. The research outcomes demonstrated how pets well may be serving as sentinels for human health, as they breathe in, ingest, or absorb the same chemicals that are in our (indoor) environments.