After a biological terrorist attack, understanding the migration of agents such as Bacillus anthracis is critical due to their deadly nature. This is important in urban settings with higher likelihood of human exposure and a large fraction of impervious materials contributing to pollutant washoff. The study goals were to understand the removal of spores from urban surfaces under different rainfall conditions, to compare washoff of two B. anthracis surrogate spores, and to compare two empirical fits for the first flush of spores from small areas. Concrete and asphalt were inoculated with either Bacillus atrophaeus or Bacillus thuringiensis kurstaki spores and exposed to simulated rainfall. The study assessed goodness-of-fit for the Storm Water Management Model (SWMM)'s exponential washoff function compared to an alternative two-stage exponential function. The highest average washoff of spores was 15% for an hour-long experiment. Spore washoff was not significantly different for the two spore types, but there were significant differences in washoff from asphalt versus concrete with more occurring from asphalt. Average kinetic energy of the storm event impacted washoff from asphalt, but not concrete. The two-stage function had a better goodness-of-fit than the SWMM exponential function. As such, emergency responders should be aware that the spread of contamination is impacted by the droplet characteristics of the storm event and the surface material type in the contaminated area; modelers should be aware that different data-fitting approaches may be more appropriate for first-flush calculations of small washoff areas than those used for continuous long-term simulation of large subcatchments.