The development of new materials for performing photocatalytic processes to remove contaminants is an interesting and important research line due to the ever-increasing number of contaminants on our planet. In this sense, we developed a layered double hydroxide material based on Zn and Cr, which was transformed into the corresponding oxide by heat treatment at 500 °C. Both materials were widely characterized for their elemental composition, and structural, morphological, optical and textural properties using several experimental techniques such as x-ray diffraction, x-ray photoelectron spectroscopy, scanning and transmission electron microscopy, Fourier transform infrared spectroscopy, UV-vis spectroscopy and physisorption techniques. In addition, the photocatalytic activity of both materials was analysed. The calcined one showed interesting photocatalytic activity in photodegradation tests using crystal violet dye. The operational parameters for the photocatalytic process using the calcined material were optimised, considering the pH, the initial concentration of the dye, the catalyst load, and the regeneration of the catalyst. The catalyst showed good photocatalytic activity, reaching a degradation of 100% in the optimised conditions and showing good performance after five photodegradation cycles.