Given positive integers $k$ and $n$, we present methods to construct all groups of order at most $n$ that contain a Cayley set of size $k$, and to enumerate the Cayley sets of order $k$ in a given group, up to the action of the automorphism group. We use these methods to generate complete lists of pairwise nonisomorphic 3-valent Cayley graphs with at most 5000 vertices and 4-valent Cayley graphs with at most 1025 vertices.