This chapter details how plasma treatments can be used to tailor the wettability of polymers. A plasma is an excited gas, and exposure of a polymer to a plasma discharge generally results in an enhancement in surface energy and associated with this is an increase in wettability. The effect however can be short lived due to hydrophobic recovery. In this review the use of both low and atmospheric plasmas for the activation of polymers will be discussed, as will the use of these plasmas for the deposition of plasma polymerised coatings. The latter can be used to produce polymer surfaces with tailored functionalities, thus achieving stable water contact angles ranging from superhydrophilic to superhydrophobic, as required.This review briefly introduces plasmas and plasma processing and includes an overview of typical plasma treatment sources. This is followed by a review of the use of plasma discharges to treat polymers and in particular to enhance their surface energy, which is important for example in achieving enhanced adhesive bond strength. The final section of this chapter focuses on the deposition of plasma polymerised coatings and how these can be used to tailor both surface chemistry and morphology. Thus the wettability of polymer surfaces can be controlled.