Plasma-based methods remain an important tool for the surface modification of materials, providing tailored surface properties while the bulk material properties remain unchanged. Plasma-based surface modification methods that have been used in the context of biomedical applications range from simple gas treatments to sophisticated plasma polymer-based coatings and interlayers. The surface treatments and coatings, which are easily transferable between substrate materials in many cases, can improve the biocompatibility and provide outstanding control over biointerfacial interactions in applications such as cell culture tools, biosensors and implantable medical devices. Herein, the current use of plasma-based methods aiming at the control of cell-material interactions is reviewed. The current knowledge is critically assessed and likely future developments are suggested.