We aimed to identify high-priority organophosphorus flame retardants for action and research. We thus critically reviewed literature between 2000 and 2019 investigating organophosphorus flame retardants’ presence indoors and human exposure in Europe, as well as epidemiological evidence of human effects. The most concentrated compounds indoors were tris(2-butoxyethyl)phosphate (TBOEP), tris(1-chloro-2-propyl)phosphate (TCIPP), tris(2,3-dichloropropyl)phosphate (TDCIPP). TBOEP and TCIPP were the most consistently detected compounds in humans’ urine, hair or breast milk as well as tris (butyl) phosphate (TNBP) and tris (phenyl) phosphate (TPHP). Notably, epidemiological evidence concerned reprotoxicity, neurotoxicity, respiratory effects and eczema risk for TDCIPP, eczema increase for TBOEP, and neurodevelopmental outcomes for Isopropylated triarylphosphate isomers (ITPs). Given the ubiquitous presence indoors and the prevalence of exposure, the growing health concern seems justified. TDCIPP and TPHP seem to be of particular concern due to a high prevalence of exposure and epidemiological evidence. TBOEP and TNBP require epidemiological studies regarding outcomes other than respiratory or dermal ones.