Full-angle spatial compounding (FASC) is a concept for pulse-echo imaging using an ultrasound tomography (UST) system. With FASC, resolution is increased and speckles are suppressed by averaging pulse-echo data from 360°. In vivo investigations have already shown a great potential for 2-D FASC in the female breast as well as for finger-joint imaging. However, providing a small number of images of parallel cross-sectional planes with enhanced image quality is not sufficient for diagnosis. Therefore, volume data (3-D) is needed. For this purpose, we further developed our UST add-on system to automatically rotate a motorized array (3-D probe) around the object of investigation. Full integration of external motor and ultrasound electronics control in a custom-made program allows acquisition of 3-D pulse-echo RF datasets within 10 min. In case of breast cancer imaging, this concept also enables imaging of near-thorax tissue regions which cannot be achieved by 2-D FASC. Furthermore, moldings made of polyvinyl alcohol hydrogel (PVA-H) have been developed as a new acoustic coupling concept. It has a great potential to replace the water bath technique in UST, which is a critical concept with respect to clinical investigations. In this contribution, we present in vivo results for 3-D FASC applied to imaging a female breast which has been placed in a PVA-H molding during data acquisition. An algorithm is described to compensate time-of-flight and consider refraction at the water-PVA-H molding and molding-tissue interfaces. Therefore, the mean speed of sound (SOS) for the breast tissue is estimated with an image-based method. Our results show that the PVA-H molding concept is applicable and feasible and delivers good results. 3-D FASC is superior to 2-D FASC and provides 3-D volume data at increased image quality.