The intriguing photophysical mechanisms of low-dimensional metal-halide hybrids are still elusive. This study investigates the optical properties and photophysical mechanisms of (C6H8N2)2ZnBr2 and (C7H10N2)CuBr2 crystals. The former shows variable emission due to π-conjugation and intramolecular halogen-hydrogen bonds, while the latter exhibits a broad, temperature-sensitive emission from self-trapped excitons.