Uracil compounds participate in a wide range of biological activities; however, reports on their synthesis using heterogeneous catalysts are scarce. In this work, the multicomponent synthesis of uracil derivatives assisted by layered double hydroxides (LDH) was studied under green chemistry conditions. The incorporation of Ni2+ or Co2+ was successfully performed by co-precipitation method. The yields to uracil derivatives are associated with the presence of weak basic sites and a better interaction of the reagents when the reaction is carried out in solvent-free conditions. The reaction pathway involves the formation of an enone between benzaldehyde and ethyl cyanoacetate, and subsequent reaction with urea, which is assisted by the presence of a basic catalyst. The scope of this synthesis is illustrated with nine examples.