Porous nanomaterials with high surface area, tunable porosity, and large mesopores have recently received particular attention in cancer therapy and imaging. Introduction of additional pores to nanostructures not only endows the tunability of optoelectronic and optical features optimal for tumor treatment, but also modulates the loading capacity and controlled release of therapeutic agents. In recognition, increasing efforts have been made to fabricate various porous nanomaterials and explore their potentials in oncology applications. Thus, a systematic and comprehensive summary is necessary to overview the recent progress, especially in last ten years, on the development of various mesoporous nanomaterials for cancer treatment as theranostic agents. While outlining their individual synthetic mechanisms after a brief introduction of the structures and properties of porous nanomaterials, the current review highlighted the representative applications of three main categories of porous nanostructures (organic, inorganic, and organic-inorganic nanomaterials). In each category, the synthesis, representative examples, and interactions with tumors were further detailed. The review was concluded with deliberations on the key challenges and future outlooks of porous nanostructures in cancer theranostics.