Reservoir Computing first emerged as an efficient mechanism for training recurrent neural networks and later evolved into a general theoretical model for dynamical systems. By applying only a simple training mechanism many physical systems have become exploitable unconventional computers. However, at present, many of these systems require careful selection and tuning by hand to produce usable or optimal reservoir computers. In this thesis we show the first steps to applying the reservoir model as a simple computational layer to extract exploitable information from complex material substrates. We argue that many physical substrates, even systems that in their natural state might not form usable or "good" reservoirs, can be configured into working reservoirs given some stimulation. To achieve this we apply techniques from evolution in materio whereby configuration is through evolved input-output signal mappings and targeted stimuli.
In preliminary experiments the combined model and configuration method is applied to carbon nanotube/polymer composites. The results show substrates can be configured and trained as reservoir computers of varying quality. It is shown that applying the reservoir model adds greater functionality and programmability to physical substrates, without sacrificing performance. Next, the weaknesses of the technique are addressed, with the creation of new high input-output hardware system and an alternative multi-substrate framework. Lastly, a substantial effort is put into characterising the quality of a substrate for reservoir computing, i.e its ability to realise many reservoirs. From this, a methodological framework is devised. Using the framework, radically different computing substrates are compared and assessed, something previously not possible. As a result, a new understanding of the relationships between substrate, tasks and properties is possible, outlining the way for future exploration and optimisation of new computing substrates.