Let \(\Gamma = (V, E)\) be a graph and a, b nonnegative integers. An (a, b)-regular set in \(\Gamma \) is a nonempty proper subset D of V such that every vertex in D has exactly a neighbours in D and every vertex in \(V{\setminus }D\) has exactly b neighbours in D. A (0, 1)-regular set is called a perfect code, an efficient dominating set, or an independent perfect dominating set. A subset D of a group G is called an (a, b)-regular set of G if it is an (a, b)-regular set in some Cayley graph of G, and an (a, b)-regular set in a Cayley graph of G is called a subgroup (a, b)-regular set if it is also a subgroup of G. In this paper, we study (a, b)-regular sets in Cayley graphs with a focus on (0, k)-regular sets, where \(k \ge 1\) is an integer. Among other things, we determine when a non-trivial proper normal subgroup of a group is a (0, k)-regular set of the group. We also determine all subgroup (0, k)-regular sets of dihedral groups and generalized quaternion groups. We obtain necessary and sufficient conditions for a hypercube or the Cartesian product of n copies of the cycle of length p to admit (0, k)-regular sets, where p is an odd prime. Our results generalize several known results from perfect codes to (0, k)-regular sets.