Single‐atom catalysts (SACs) are desirable in environmental catalysis due to environmental friendliness, structural stability, and maximum utilization of active metal sites. Extensive research has compared the catalytic performance between SACs with different single‐atom metals. However, their catalytic performance is also highly dependent on the supports, which play an important role in modulating the local coordination environment of SACs. Unfortunately, a comprehensive review that systematically discusses the relationship between supports and the coordination environment, as well as their combined effects on environmental catalysis is scare. In this review, three widely investigated environmental applications including advanced oxidation processes (AOPs), mainly Fenton and Fenton‐like reactions, and nitrate reduction reaction (NO3RR) are focused. By correlating characterization results, catalytic performances, and computational results, the combined effects of supports and coordination environments on the catalytic reactivity of SACs are examined in detail, from which the origin of the catalytic pathways of AOPs as well as NO3RR is attempted to reveal. Finally a look forward for potential opportunities and challenges of SACs for on‐demand environmental applications, is provided.