<p>This review highlights the hybridization of urea with smectites, focusing on synthesis methods, structural characterizations, and diverse applications of urea/smectite hybrids. Due to the swelling properties and cation exchange capacity of smectites, urea can be intercalated into the interlayer space using three main approaches: solution-based methods, mechanochemical activation, and solvent-free mixing with molten urea complexes. Key synthetic parameters—such as urea-to-smectite mass ratio, concentration, reaction time, milling technique, and the use of urea-metal complexes—are discussed in relation to the interactions between urea and smectites, as well as the resulting structural modifications. These interactions are crucial for enhancing urea retention and controlled release, enabling applications across agriculture, environmental protection, engineering, and medicine.</p> Graphical abstract <p>The hybridization urea with smectites and applications.</p>