Poly(amidoamine) (PAMAM) dendrimers, as a family of synthetic macromolecules with highly branched interiors, abundant surface functional groups, and well-controlled architecture, have received immense scientific and technological interests for a range of biomedical applications, in particular cancer nanomedicine. However, due to the drawbacks of single-generation dendrimers with a quite small size (e.g., generation 5 (G5) PAMAM dendrimer has a size of 5.4 nm) such as limited drug loading capacity, restricted tumor passive targeting based on enhanced permeability and retention effect, and lack of versatility to render them with stimuli-responsiveness, superstructured dendrimeric nanoconstructs (SDNs) have been designed to break through these obstacles in their applications in cancer nanomedicine. Here, we review the recent advances related to the creation of SDNs such as dendrimer dumbbells, core–shell tecto dendrimers, dendrimer nanoclusters (NCs), dendrimer nanogels and dendrimer-templated hybrid NCs, and how these SDNs have been designed as nanoplatforms for different biomedical applications related to cancer nanomedicine including MR imaging, drug/gene delivery, combination therapy and theranostics. This review concisely describes the latest key developments in the field and also discusses the possible challenges and perspectives for translation applications.