Materials offering the ability to change their characteristics in response to presented stimuli have demonstrated application in the biomedical arena, allowing control over drug delivery, protein adsorption and cell attachment to materials. Many of these smart systems are reversible, giving rise to finer control over material properties and biological interaction, useful for various therapeutic treatment strategies. Many smart materials intended for biological interaction are based around pH or thermo-responsive materials, although the use of magnetic materials, particularly in neural regeneration, has increased over the past decade. This review draws together a background of literature describing the design principles and mechanisms of smart materials. Discussion centres on recent literature regarding pH-, thermo-, magnetic and dual responsive materials, and their current applications for the treatment of neural tissue.