Co/Cu/Co pseudo-spin-valves (PSVs) were deposited with different buffer and capping layers on natiral Si wafers using magnetron sputtering. Improved magnetoresistance (MR) performance was achieved with Fe buffer due to induced anisotropy with sharp magnetization reversal, high MR value (9.2%), and enhanced field sensitivity (>2.0%/Oe) at low switching field (20 Oe). The magnetization reversal of the PSVs with Cr/Cu buffer was found to be dependent on the Cu spacer thickness showing oscillations. The PSVs with Fe buffer showed excellent properties and sharp switching from 5 K to 300 K. The overall switching behavior is strongly influenced by the capping layer by affecting magnetic coupling between the two Co layers. The MR values of the PSVs were accurately interpreted within a model based on first principles solution to the Boltzmann transport equations calculations.