Cellular organelles, such the cytomembrane, lysosome, mitochondrion, Golgi apparatus, the endoplasmic reticulum, and nucleus, play important roles in the normal function of cells. Organelle-targeting bioimaging can aid our understanding of how organelles function, while the development of organelle-targeting therapy could deliver treatment for a variety of diseases. Possessing important advantages such as their photophysical properties, cytotoxicity, and cellular uptake mechanisms, metal complexes for organelle-targeting bio-applications have attracted increasing attention in recent years. In this review, organelle-targeting regulating strategies, and the characteristics of organelle-targeting metal complexes as well as their bio-applications are summarized. Moreover, the existing opportunities/challenges of organelle targeting are outlined and emphasized to inspire the design of a new generation of organelle-targeting metal complexes.