The metal-based drugs represented by cisplatin, carboplatin, and oxaliplatin, prevail in cancer treatment, whereas new therapeutics are extremely slow to step into the clinic. Poor pharmacokinetics, multidrug resistance, and severe side effects greatly limit the development of metal-based anticancer drugs. The robustness and modular composition of supramolecular coordination complexes allow for the incorporation of novel diagnostic and therapeutic modalities, showing promising potentials for precise cancer theranostics. In this mini review, we highlight the recent advances in the development of supramolecular coordination complexes as diagnostic and therapeutic agents. The key focuses of these reports lie in searching sophisticated coordination ligands and nanoformulations that can potentially solve the issues faced by current metal-based drugs including imaging, resistance, toxicity, and pharmacological deficiencies.