The use of nanomaterials is an exciting prospect to facilitate radiotherapy delivery based on molecular targeting of tumors. This molecular targeted radiotherapy approach involves the use of radioligands – radioactive isotopes that are chemically linked to tumor‐binding ligands – to ensure that radiation damage is delivered accurately and efficiently to tumor cells while sparing normal tissues. Although the use of nanomaterials has been well summarized for passive cancer radiotherapy, a clinical take on modern molecular targeted radioligand applications is yet to be reviewed. In this review, we will firstly discuss the innovative design of nanomaterials in relation to pre‐clinical molecular targeted radioligand therapy. As we identify a current lack of clinical nanomaterial‐based radiotherapy across various tumor types, we then provide our insights on related challenges and strategies to clinically translate innovative nanomaterial technologies to aid in driving molecular targeted radioligand therapies.