In this paper, a pillared layer mixed ligand metal–organic framework (MOF), namely, DMOF-1–Zn was synthesized via anodic dissolution in an electrochemical cell. The influence of different reaction parameters such as solvent, additive and current density on the textural properties of the MOF obtained were investigated. The characterization of the samples involved powder X-ray diffraction, infrared Fourier transform spectroscopy, and field emission scanning electron microscopy. Moreover, the electrochemical route was successfully combined with a coordination modulation approach to prepare specific morphology at the nano-scale. The main advantages of electrosynthesis are the shorter synthesis time, the milder conditions, the facile synthesis of MOF nanostructures and the morphology tuning.