Substrates that compute using vibration rather than electricity offer the potential of creating and deploying computers into electronics-denying environments. Another advantage of these materials is that some of them can compute multiple functions in the same place and at the same time, providing computational results at different frequencies. These so-called polycomputational materials may eventually compete with more traditional computers in terms of computational density because there is no currently known upper bound on how many functions can be simultaneously computed by a vibrational substrate. However, three challenges remain for polycomputational materials: how to ensure that the different functions are computed independently; developing evolutionary algorithms that allow for embedding increasingly more functions into these materials in silico; and validating the evolved in silico materials as physical materials. Here we report progress on all three of these issues.