We have found a novel method for increasing the giant magnetoresistance (GMR) of Co/Cu spin valves with the use of oxygen. Surprisingly, spin valves with the largest GMR are not produced in the best vacuum. Introducing5×10−9Torr(7×10−7Pa) into our ultrahigh vacuum deposition chamber during spin-valve growth increases the GMR, decreases the ferromagnetic coupling between magnetic layers, and decreases the sheet resistance of the spin valves. It appears that the oxygen may act as a surfactant during film growth to suppress defects and to create a surface which scatters electrons more specularly. Using this technique, bottom spin valves and symmetric spin valves with GMR values of 19.0&percent; and 24.8&percent;, respectively, have been produced. These are the largest values ever reported for such structures. ©1997 American Institute of Physics.