Heterogeneous chemical cycles of pyrogenic nitrogen and halides influence tropospheric ozone and affect the stratosphere during extreme Pyrocumulonimbus (PyroCB) events. We report field‐derived N2O5 uptake coefficients, γ(N2O5), and ClNO2 yields, φ(ClNO2), from two aircraft campaigns observing fresh smoke in the lower and mid troposphere and processed/aged smoke in the upper troposphere and lower stratosphere (UTLS). Derived φ(ClNO2) varied across the full 0–1 range but was typically <0.5 and smallest in a PyroCB (<0.05). Derived γ(N2O5) was low in agricultural smoke (0.2–3.6 × 10 3), extremely low in mid‐tropospheric wildfire smoke (0.1 × 10 3), but larger in PyroCB processed smoke (0.7–5.0 × 10 3). Aged biomass burning aerosol in the UTLS had a higher γ(N2O5) of 17 × 10 3 that increased with sulfate and liquid water, but that was 1–2 orders of magnitude lower than values for aqueous sulfuric aerosol used in stratospheric models. Plain Language Summary The injection of reactive material into Earth's atmosphere from fires affects atmospheric composition at regional and hemispheric scales. Reported stratospheric ozone depletion during extreme events, such as the 2020 Australian wildfires, illustrates one example of fire impacts and the role of heterogeneous (gas‐particle) processes. We report field quantification of rates and product yields from