We investigate the spectrum for frames with block size four, and discuss several applications to the construction of other combinatorial designs. Our main result is that a frame of type hu, having blocks of size four, exists if and only if u ≥ 5, h ≡ 0 mod 3 and h(u − 1) ≡ 0 mod 4, except possibly where (i) h = 9 and u ∈ {13, 17, 29, 33, 93, 113, 133, 153, 173, 193}; (ii) h ≡ 0 mod 12 and u ∈ {...