Calibration of local, regional or global allometric equations to estimate biomass at the tree level constitutes a significant burden on projects aiming at reducing Carbon emissions from forest degradation and deforestation. The objective of this contribution is to assess the precision and accuracy of Terrestrial Laser Scanning (TLS) for estimating volumes and above‐ground biomass (AGB) of the woody parts of tropical trees, and for the calibration of allometric models. We used a destructive dataset of 61 trees, with diameters and AGB of up to 186.6 cm and 60 Mg respectively, which were scanned, felled and weighed in the semi‐deciduous forests of eastern Cameroon. We present an operational approach based on available software allowing the retrieving of TLS volume with low bias and high accuracy for large tropical trees. Edition of the obtained models proved necessary, mainly to account for the complexity of buttressed parts of tree trunks, which were separately modelled through a meshing approach, and to bring a few corrections in the topology and geometry of branches, thanks to the amapstudio‐scan software. Over the entire dataset, TLS‐derived volumes proved highly reliable for branches larger than 5 cm in diameter. The volumes of the remaining woody parts estimated for stumps, stems and crowns as well as for the whole tree proved very accurate (RMSE below 2.81% and R² above of .98) and unbiased. Once converted into AGB using mean local‐specific wood density values, TLS estimates allowed calibrating a biomass allometric model with coefficients statistically undistinguishable from those of a model based on destructive data. The Unedited Quantitative Structure Model (QSM) however leads to systematic overestimations of woody volumes and subsequently to significantly different allometric parameters. We can therefore conclude that a non‐destructive TLS approach can now be used as an operational alternative to traditional destructive sampling to build the allometric equations, although attention must be paid to the quality of QSM model adjustments to avoid systematic bias.