This work provides an evaluation of an ultrasound-assisted, combined extraction, centrifugation and ultrafiltration process for the optimal recovery of polyphenols. A purple sweet potato (PSP) extract has been obtained using ultrasonic circulating extraction equipment at a power of 840 W, a frequency of 59 kHz and using water as solvent. Extract ultrafiltration, using polyethersulfone (PES), was carried out for the recovery of polyphenol, protein and anthocyanin. Pre-treatment, via the centrifugation of purple sweet potato extract at 2500 rpm over 6 min, led to better polyphenol recovery, with satisfactory protein removal (reused for future purposes), than PSP extract filtration without centrifugation. Results showed that anthocyanin was efficiently recovered (99%) from permeate. The exponential model fit well with the experimental ultrafiltration data and led to the calculation of the membrane’s fouling coefficient. The optimization of centrifugation conditions showed that, at a centrifugation speed of 4000 rpm (1195× g) and duration of 7.74 min, the optimized polyphenol recovery and fouling coefficient were 34.5% and 29.5 m−1, respectively. The removal of proteins in the centrifugation process means that most of the anthocyanin content (90%) remained after filtration. No significant differences in the intensities of the HPLC-DAD-ESI-MS2 peaks were found in the samples taken before and after centrifugation for the main anthocyanins; peonidin-3-feruloylsophoroside-5-glucoside, peonidin-3-caffeoyl-p-hydroxybenzoylsophoroside-5-glucoside, and peonidin-3-caffeoyl-feruloyl sophoroside-5-glucoside. This proves that centrifugation is an efficient method for protein removal without anthocyanin loss. This study considers this process an ultrasound-assisted extraction-centrifugation-ultrafiltration for purple sweet potato valorization in “green” technology.