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A family of Ruddlesden–Popper (<i>n</i> = 1) layered perovskite-related phases, Az₂PbCl<i>_x</i>Br_4−<i>x</i> with composition 0 ≤ <i>x</i> ≤ 4 were obtained using mechanosynthesis. These compounds are isostructural with K₂NiF₄ and therefore adopt the idealised <i>n</i> = 1 Ruddlesden–Popper structure. A linear variation in unit cell volume as a function of anion average radius is observed. A tunable bandgap is achieved, ranging from 2.81 to 3.43 eV, and the bandgap varies in a second-order polynomial relationship with the halide composition.