The distributions of organophosphate flame retardants (OPFRs) in various size fractions of indoor dust samples from homes (H; n = 18) and building material markets (B; n = 7) in the Rhine/Main region of Germany were investigated. Three particle size fractions (F1: 150–200 μm, F2: 63–150 μm, and F3: <63 μm) and bulk dust (BD) subsamples (<200 μm) of each sample were analyzed for 10 OPFRs. On average, the total OPFR concentrations (∑10OPFR) in bulk dust and all three size fractions from building material markets were 133, 153, 196, and 88.0 μg/g in subsamples B-BD, B-F1, B-F2, and B-F3. These concentrations were at least five times higher than those in bulk dust and all three size fractions from homes, with values of 19.3, 17.2, 19.5, and 18.7 μg/g for subsamples H-BD, H-F1, H-F2, and H-F3, respectively. Tris(2-chloroisopropyl)phosphate (TCIPP) was the dominant congener in dust from building material markets, contributing over 91% to the ∑10OPFR of B-BD and all particle size fractions. Meanwhile, both tris(2-butoxyethyl)phosphate (TBOEP) and TCIPP were abundant in dust from homes, respectively contributing 28%–41% and 31%–43% to the ∑10OPFR of H-BD and all particle size fractions. Most of the OPFR concentrations showed no consistent trend with particle size. However, TCIPP was more likely to be enriched in F2. Microscopic examination indicated that TCIPP in indoor dust mainly originated from abraded fragments of commercial products. In contrast, TBOEP accumulated in F3, related to direct transfer of floor-care products to fine dust particles. The concentrations of OPFRs were not significantly correlated with total organic carbon contents in any particle size fraction. However, evaluation of their mass contributions showed that more than 85% of OPFRs accumulated in particles smaller than 150 μm, indicating that this particle size fraction is most suitable for monitoring of OPFRs. Display omitted •OPFR concentrations in dust from homes and building material markets were compared.•Building material markets had higher OPFR levels than private homes.•TCIPP was typically enriched in the intermediate dust fraction F2 (63–150 μm in size).•TBOEP tended to accumulate in the finest dust fraction F3 (<63 μm in size).•Monitoring of OPFRs in indoor dust particles < 150 μm in size is recommended. This study explores the contribution of different dust size fractions to OPFR contamination in homes and building material markets.