Indoor pollution poses a serious threat to human health. Plants represent a sustainable but underexploited solution to enhance indoor air quality. However, the current selection of plants suitable for indoors fails to consider the physiological processes and mechanisms involved in phytoremediation. Therefore, the capacity of plants to remove indoor air pollutants through stomatal uptake (absorption) and non-stomatal deposition (adsorption) remains largely unknown. Moreover, the effects of the indoor plant-associated microbiome still need to be fully analyzed. Here, we discuss how a combination of the enhanced phytoremediation capacity of plants together with cutting-edge air-cleaning and smart sensor technologies can improve indoor life while reducing energy consumption.