The progress toward structure refinement of solid-type uniformly 1 3 C enriched ([U- 1 3 C]) chlorophyll-containing biological preparations is summarised. Solid state carbon chemical shifts of aggregated [U- 1 3 C] bacteriochlorophyll (BChl) c in intact chlorosomes of Chlorobium tepidum and in [U- 1 3 C] BChl c aggregates were determined by the application of homonuclear ( 1 3 C 1 3 C) magic angle spinning (MAS) NMR dipolar correlation spectroscopy. It was found that the arrangement of BChl c molecules in the chlorosomes and in the aggregates is highly similar, which provides convincing evidence that self-organisation of the BChl c is the main mechanism to support the structure of the chlorosomes. Additionally, high field 2-D ( 1 H 1 3 C) and 3-D ( 1 H 1 3 C 1 3 C) dipolar correlation spectroscopy was applied to determine solid state proton chemical shifts of aggregated [U- 1 3 C] BChl c in intact chlorosomes. From the high-field assignments, evidence is found for the existence of at least two well-defined interstack arrangements.