The evaluation and control of the cellular response to substrate materials is important for a wide range of regenerative medicine applications including implants, biomaterial devices and biosensors. Gradient surfaces provide a simple and fast method for determining optimal surface conditions for cellular responses such as attachment and growth. This chapter presents an overview of high-throughput techniques available for the optimisation of cell material interactions with particular emphasis on surface topographical and chemical gradients. The gradient approaches presented throughout this chapter are expected to become useful tools for researchers that are aiming to optimise advanced materials for a variety of biomedical applications.