Due to the inherent complexity of environmental problems, especially water and air pollution, the utility of single-function environmental nanomaterials used in conventional and unconventional environmental treatment technologies are gradually reaching their limits. Intelligent nanomaterials with environmentally-responsive functionalities have shown potential to improve the performance of existing and new environmental technologies. By rational design of their structures and functionalities, intelligent nanomaterials can perform different tasks in response to varying application scenarios for the purpose of achieving the best performance. This review offers a critical analysis of the design concepts and latest progresses on the intelligent environmental nanomaterials in filtration membranes with responsive gates, materials with switchable wettability for selective and on-demand oil/water separation, environmental materials with self-healing capability, and emerging nanofibrous air filters for PM2.5 removal. We hope that this review will inspire further research efforts to develop intelligent environmental nanomaterials for the enhancement of the overall quality of environmental or human health.