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The mechanical and chemical properties of diamond and diamond-like carbon (DLC) coatings make them very suitable materials for improving the long-term performance of invasive electrode systems used in brain–computer interfaces (BCIs). We have performed in vitro testing to demonstrate methods for spatially directing neural cell growth and limiting the detrimental attachment of cells involved in the foreign body response on boron-doped diamond and DLC. Inkjet-printing, laser micro-machining, and stencil-assisted patterning techniques were used to control neuronal adhesion and modify inflammatory cell attachment. This work presents micro-tailored materials that could be used to improve the long-term quality of recorded signals from neural-electronic interfaces.