Understanding per- and polyfluoroalkyl substances (PFAS) mass distribution in surface and groundwater systems can support source prioritization, load reduction, and water management. Thirteen sites within an urban catchment were sampled utilizing a time-of-travel sampling approach to minimize the influence of subdaily fluctuations in mass from PFAS point sources and to quantify PFAS and ancillary chemical loads from various PFAS sources. A larger increase in perfluoroalkyl sulfonate (PFSA) loads (8 to 11 μg/s, up to 618%) than in perfluoroalkyl carboxylate (PFCA) loads (no change to 3.4 μg/s, up to 122%) was observed at sites below tributaries influenced by military bases with known groundwater discharge. Point discharges from two sewage treatment plants (STPs) resulted in increases in PFCA and PFSA loads that were similar (6 and 10 μg/s respectively) below the first STP and greater for PFCA compared to PFSA loads (23 and 13 μg/s respectively) below the second STP. Overall, percent increases in total PFAS load ranged from 20 to 277% for military base inputs and 44 to 77% for STP inputs. A focus catchment that represents only 14% (76.9 km²) of the drainage area at the most downstream site (544 km²) accounted for about 70% of PFSA and 40% of PFCA loads observed at the most downstream site. Results show that by using a time-of-travel sampling approach in mixed, urban settings with several PFAS sources, it is possible to quantify stream loads from individual PFAS sources, thereby improving source attribution and providing actionable data for water-resource managers.