Bryophytes are a poorly studied group of land plants that have been used in traditional medicine as a multipurpose remedy for centuries. Due to their peculiar morphology and physiology, bryophytes synthesise a multitude of secondary metabolites with a wide range of nutraceutical and pharmaceutical activities. Research has highlighted that secondary metabolites in bryophytes can also act as antitumour agents. Several studies have shown that bryophyte extracts and pure metabolites are cytotoxic against many cancer cell lines. Interestingly, some of these molecules and their derivatives are capable of acting on a specific target in cancer cells. Some macrocyclic(bis)bibenzyls from bryophytes can inhibit P-glycoprotein, reverting multidrug resistant cancer cell phenotypes, induce depolymerization of tubulin, stimulate apoptotic pathways, and inhibit angiogenesis. This brief review aims to collect recent knowledge on secondary metabolites of bryophytes and their derivatives, which have demonstrated an interaction with different molecular processes in cancer cells.