Edge-transitive graphs of order a prime or a product of two distinct primes with any positive integer valency, and of square-free order with valency at most 7 have been classified by a series of papers. In this paper, a complete classification is given of edge-transitive Cayley graphs of square-free order with valency less than the smallest prime divisor of the order. This leads to new constructions of infinite families of both arc-regular Cayley graphs and edge-regular Cayley graphs (so half-transitive). Also, as by-products, it is proved that, for any given positive integers k, s ≥ 1 and m, n ≥ 2, there are infinitely many arc-regular normal circulants of valency 2k and order a product of s primes, and there are infinitely many edge-regular normal metacirculants of valency 2m and order a product of n primes; such arc-regular and edge-regular examples are also specifically constructed.