The requirements for non-invasive visualization and precise treatment of cancers are ongoing, demanding continuous efforts to enhance the development of potent theranostic modalities. Notably, groundbreaking advancements in nanotechnology have positioned layered double hydroxides (LDHs) at the forefront of biomedical research. LDH carriers are highly valued in medicinal applications due to their ability to integrate the benefits of multiple modalities, thus paving a promising path to clinical use. Recent breakthroughs in the rational design of theranostics have underscored the potential of gadolinium (Gd)-doped LDHs, which are particularly well-suited for the diagnosis of diseases. This review focuses on providing a comprehensive overview of the latest significant advances in Gd-LDH assemblies in cancer theranostics, with an emphasis on a bottom-up intercalation strategy, influential factors, and formulation methodologies. These aspects are crucial for researchers developing innovative intercalation processes and novel multi-component materials. Additionally, we address the kinetic inertness and colloidal stability of Gd-intercalated LDHs, which are essential for advanced theranostic applications. Finally, we present a forward-looking discussion on the challenges and future opportunities related to Gd-LDH complexes, aiming to identify the obstacles researchers encounter in advancing the clinical application of Gd-LDHs and to offer potential insights for further research. © 2024 Elsevier B.V.