Cancer is a leading cause of death in both developing and developed countries. With the increase in the average global life expectancy, it has become a major health problem and burden for most public healthcare systems worldwide. Due to the fewer side effects of natural compounds than of chemotherapeutic drugs, increasing scientific attention is being focused on the development of anti-cancer drugs derived from natural sources. Marine algae are an interesting source of functional compounds with diverse health-promoting activities. Among these compounds, polysaccharides have attracted considerable interest for many years because of their excellent anti-cancer abilities. They improve the efficacy of conventional chemotherapeutic drugs with relatively low toxicity to normal human cells. However, there are few reviews summarising the unique anti-cancer effects and underlying mechanisms of marine algae polysaccharides (MAPs). Thus, the current review focuses on updating the advances in the discovery and evaluation of MAPs with anti-cancer properties and the elucidation of their mechanisms of action, including the signalling pathways involved. This review aims to provide a deeper understanding of the anti-cancer functions of the natural compounds derived from medicinal marine algae and thereby offer a new perspective on cancer prevention and therapy with high effectiveness and safety.