A novel super-complex of photosystem I (PSI)-light-harvesting complex I (LHCI) was isolated from a siphonaceous marine green alga, Bryopsis corticulans. The super-complex contained 9-10 Lhca antennas as external LHCI bound to the core complex. The super-complex was further disintegrated into PSI core and LHCI sub-complexes, and analysis of the pigment compositions by high-performance liquid chromatography revealed unique characteristics of the B. corticulans PSI in that one PSI core contained around 14 α-carotenes and 1-2 ε-carotenes. This is in sharp contrast to the PSI core from higher plants and most cyanobacteria where only β-carotenes were present, and is the first report for an α-carotene-type PSI core complex among photosynthetic eukaryotes, suggesting a structural flexibility of the PSI core. Lhca antennas from B. corticulans contained seven kinds of carotenoids (siphonaxanthin, all-trans neoxanthin, 9'-cis neoxanthin, violaxanthin, siphonein, ε-carotene, and α-carotene) and showed a high carotenoid:chlorophyll ratio of around 7.5:13. PSI-LHCI super-complex and PSI core showed fluorescence emission peaks at 716 and 718 nm at 77 K, respectively; whereas two Lhca oligomers had fluorescence peaks at 681 and 684 nm, respectively. By comparison with spinach PSI preparations, it was found that B. corticulans PSI had less red chlorophylls, most of them are present in the core complex but not in the outer light-harvesting systems. These characteristics may contribute to the fine tuning of the energy transfer network, and to acclimate to the ever-changing light conditions under which the unique green alga inhabits.