Nanomaterials possess unique size characteristics, enabling them to cross tissue gaps, penetrate the blood-brain barrier and endothelial cells, and release drugs at the cellular level. Additionally, the surface of nanomaterials is readily functionalized, endowing them with good biocompatibility, low biotoxicity, and specific targeting. All these advantages render nanomaterials broad application prospects in tumor therapy. Pillar[5]arenes are a new category of macrocyclic host compounds featuring rich host-guest properties and diverse environmental responses. In recent years, by combining the advantages of pillar[5]arenes and nanomaterials, the application of pillar[5]arene-based nanomaterials in tumor therapy has drawn extensive attention from scientists. In this review, we summarize five distinct types of pillar[5]arene-based nanomaterials: (1) pillar[5]arene-modified inorganic nanomaterials; (2) pillar[5]arene-modified organic porous materials; (3) pillar[5]arene-modified organic/inorganic hybrid materials; (4) nanomaterials self-assembled from pillar[5]arene-based host-guest complexes; (5) nanomaterials self-assembled from amphiphilic pillar[5]arenes. Moreover, the different tumor treatment modes of these nanomaterials, including chemotherapy, photodynamic therapy, photothermal therapy, gene therapy, and multimodal synergistic therapy, are also elaborated in detail.