Cancer is a severe health menace to human beings. Chemotherapy is frequently used in clinics. However, there are many limitations with the traditionally chemical synthetic anticancer drugs. Fortunately, in recent decades, phytodrugs have contributed a lot to cancer therapy and account for more than half of the current anticancer agents in clinics. In this chapter, first of all, based on their plant source, chemical structure, and mechanism of action, the promising anticancer phytodrugs are introduced, including alkaloids, podophyllotoxin, combretastatins, and flavonoids, and the representative phytodrugs in each type are emphasized, including paclitaxel, camptothecin, teniposide, matrine, vinblastine, homoharringtonine, combretastatin, curcumin, and quercetin. Thereafter, based on the challenges in drug delivery, the promising micro/nano-carrier based systems for better delivery of these anticancer phytodrugs are described, including phytosomes, liposomes, niosomes, nanoparticles, microspheres, and emulsions. In conclusion, this review offers an insight on the expanded potential of phytodrugs toward anticancer treatment.