Giant Magnetoresistance (GMR) is reported in as-deposited Ag1−xCox (x = 0.26–0.53) films co-sputtered on Si from separate Ag and Co targets. GMR ratios (10 K Oe Maximum field) exceeding 0.50 and 0.19 at 5 and 295 K, respectively, are observed for the Ag067Co033 films deposited at ≃28 to 175 °C. The Maximum ratios of 0.55 and 0.24 occur at a substrate temperature of ≃125 °C for these films. The ratios decrease rapidly for the films deposited at temperatures > 175 °C and reduce to ≃0.15 and 0.04 at deposition temperatures >300 °C. This deposition temperature dependence of GMR ratios is interpreted in terms of the change in the spin-dependent interfacial electron scatterings due to the change in the size and number of ferromagnetic Co particles within the electron mean free path. The initial increase and the subsequent decrease in GMR ratios with increasing deposition temperature are attributed to the increase in the mean free path, and the Co and Ag particle size, respectively. Changes in mean free path are obtained from the resistivities of these films while changes in Ag and Co particles are deduced mainly from the X-ray diffraction patterns, transmission electron Micrographs, and the coercivities of these films.