Accurate activity quantification is the foundation for all methods of radiation dosimetry for molecular radiotherapy (MRT). The requirements for patient-specific dosimetry using single photon emission computed tomography (SPECT) are challenging, particularly with respect to scatter correction. In this paper data from phantom studies, combined with results from a fully validated Monte Carlo (MC) SPECT camera simulation, are used to investigate the influence of the triple energy window (TEW) scatter correction on SPECT activity quantification for [Formula: see text]Lu MRT. Results from phantom data show that; (1) activity quantification for the total counts in the SPECT field-of-view demonstrates a significant overestimation in total activity recovery when TEW scatter correction is applied at low activities ([Formula: see text]200 MBq). (2) Applying the TEW scatter correction to activity quantification within a volume-of-interest with no background activity provides minimal benefit. (3) In the case of activity distributions with background activity, an overestimation of recovered activity of up to 30% is observed when using the TEW scatter correction. Data from MC simulation were used to perform a full analysis of the composition of events in a clinically reconstructed volume of interest. This allowed, for the first time, the separation of the relative contributions of partial volume effects (PVE) and inaccuracies in TEW scatter compensation to the observed overestimation of activity recovery. It is shown, that even with perfect partial volume compensation, TEW scatter correction can overestimate activity recovery by up to 11%. MC data is used to demonstrate that even a localized and optimized isotope-specific TEW correction cannot reflect a patient specific activity distribution without prior knowledge of the complete activity distribution. This highlights the important role of MC simulation in SPECT activity quantification.