Nanotechnology has emerged as highly promising tools for cancer therapy. In comparison to traditional therapeutic methods (e.g., chemotherapy and radiotherapy) generally involving limited specificity and undesired side effects, nanomaterials (e.g., magnetic nanoparticles, carbon-based nanomaterials, and porous silicon, etc.)-based nanoagents and therapeutic strategies significantly facilitate the improvement of therapeutic efficacy and reduce the toxic side effect. In particular, silicon nanomaterials featuring large surface-to-volume ratio and abundant surface chemistry open up completely new avenues for design of novel silicon-based nanoagents with large drug-loading capacity and high tumor-targeting efficacy. In the past decade, porous silicon (pSi) has been widely employed as high-performance delivery systems for different types of therapeutic drug molecules, proteins, and genes, aiming at improved therapeutic efficacy and reduced toxic side effect. The pSi can be also functionalized with photosensitizers, radiosensitizers, or heat producers, which are efficacious for phototherapy or radiotherapy of cancer. On the other hand, silicon nanowires (SiNWs) and SiNWsbased nanohybrids (e.g., gold nanoparticles/nanospheres-coated SiNWs), serving as novel classes of drug nanocarriers and hyperthermia nanoagents, have recently been explored for in vitro and in vivo cancer therapy with encouraging therapeutic outcomes.