Two-level Cretan matrices are orthogonal matrices with two elements, x and y. At least one element per row and column is 1 and the other element has modulus ≤ 1. These have been studied in the Russian literature for applications in image processing and compression. Cretan matrices have been found by both mathematical and computational methods but this paper concentrates on mathematical solutions for the first time. We give, for the first time, families of Cretan matrices constructed using the incidence matrix of a symmetric balanced incomplete block design and Hadamard related difference sets.