Oxygen cycling of Sr2Fe2–xMoxO6–δ (SFMO) samples allows the resistivity and low‐field magnetoresistance (LFMR) to be precisely cycled. TEM shows that the change in resistivity with oxygen is not only a consequence of the change in oxygen stoichiometry of SFMO, but also a concomitant change in the Fe/Mo ratio in SFMO. The figure shows the change in MR and resistivity (values in mΩ cm above the data points for samples D1–D7) with increasing post‐annealing time.