Environmentally attractive synthetic routes are studied for the synthesis of MgAl-layered double hydroxides (LDHs) incorporating a series of organic dicarboxylate anions. The reaction conditions are systematically explored to ascertain the effect of acid chain length and layer charge (i.e. Mg/Al ratio). The materials are characterised by powder X-ray diffraction, scanning electron microscopy, infra-red spectroscopy and thermal methods. The effect of reaction conditions on product purity and the packing arrangement of the intercalated organic molecules is reported, with impurity free organo-LDHs observed at Mg/Al = 2 and increased interlayer packing as Mg/Al approaches 1.