Layered double hydroxides (LDHs) and their derived mixed oxides are emerging as a promising class of biocompatible inorganic lamellar nanomaterials. The detailed structure and textural characteristics of the synthesized LDH-based materials were examined using X-ray diffraction, Fourier transform infrared spectroscopy, and N2 adsorption/desorption isotherm. This study explored the removal efficiency of pharmaceutical tolperisone hydrochloride (TLP), as well as the herbicides quinmerac (QUI) and clomazone (CLO) from water, using dried and calcined LDH-based photocatalysts under simulated solar irradiation and UV irradiation. A higher removal efficiency was observed using UV irradiation, for all substrates. The most effective removal was achieved using ZnAl photocatalysts thermally treated at 100 °C (ZnAl 100) and 500 °C (ZnAl 500). The highest removal rates were observed in the TLP/ZnAl 100 and QUI/ZnAl 100 systems, achieving ~79% and ~86% removal after 75 min of treatment under UV. In contrast, the CLO/ZnAl 100 and CLO/ZnAl 500 systems achieved ~47% removal of CLO. Furthermore, this study investigated the role of reactive species to elucidate the mechanisms of photodegradation under UV. It was found that in the degradation of TLP and QUI in the presence of ZnAl 100 and ZnAl 500, the superoxide anion radical played the most important role.