Large trees are disproportionately important in terms of their above ground biomass (AGB) and carbon storage, as well as their wider impact on ecosystem structure. They are also very hard to measure and so tend to be underrepresented in measurements and models of AGB. We show the first detailed 3D terrestrial laser scanning (TLS) estimates of the volume and AGB of large coastal redwood Sequoia sempervirens trees from three sites in Northern California, representing some of the highest biomass ecosystems on Earth. Our TLS estimates agree to within 2% AGB with a species-specific model based on detailed manual crown mapping of 3D tree structure. However TLS-derived AGB was more than 30% higher compared to widely-used general (non species-specific) allometries. We derive an allometry from TLS that spans a much greater range of tree size than previous models and so is potentially better-suited for use with new Earth Observation data for these exceptionally high biomass areas. We suggest that where possible, TLS and crown mapping should be used to provide complementary, independent 3D structure measurements of these very large trees.