Single-photon emission computed tomography (SPECT) allows the three-dimensional visualization of radioactivity within the human body and is widely used for clinical purposes. In SPECT, image quality is compromised by several factors including photon attenuation, photon scatter, the partial volume effect, and motion artefacts. These variables also confound the capacity of SPECT to quantify the concentration of radioactivity within given volumes of interest in absolute units, e.g. as kilobecquerels per cubic centimetre. In the last decade, considerable technical progress has been achieved in SPECT image reconstruction, involving, in particular, the development of iterative image reconstruction techniques. Furthermore, hybrid cameras integrating a SPECT camera with an X-ray CT scanner have become commercially available. These systems allow the acquisition of SPECT and CT datasets registered to each other with a high anatomical accuracy. First studies have shown that iterative SPECT image reconstruction techniques incorporating information from SPECT/CT image datasets greatly increase the accuracy of SPECT in quantifying radioactivity concentrations in phantoms and also in humans. This new potential of SPECT may improve not only diagnostic accuracy, but also dosimetry for internal radiotherapy.