Red algae contain two types of light-harvesting antenna systems, the phycobilisomes and chlorophyll a binding polypeptides (termed Lhcr), which expand the light-harvesting capacity of the photosynthetic reaction centers. In this study, photosystem I (PSI) and its associated light-harvesting proteins were isolated from the red alga Cyanidioschyzon merolae. The structural and functional properties of the largest PSI particles observed were investigated by biochemical characterization, mass spectrometry, fluorescence emission and excitation spectroscopy, and transmission electron microscopy. Our data provide strong evidence for a stable PSI complex in red algae that possesses two distinct types of functional peripheral light-harvesting antenna complex, comprising both Lhcr and a PSI-linked phycobilisome sub-complex. We conclude that the PSI antennae system of red algae represents an evolutionary intermediate between the prokaryotic cyanobacteria and other eukaryotes, such as green algae and vascular plants.