In this work, the use of ultrasound energy for chromium removal from residual tannery leather was investigated. The following parameters were evaluated: complexation temperature (60–90 °C), chromium/complexant molar ratio (1:0 to 1:6), complexation time (30–120 min), washing steps (1–14), washing temperature (25–80 °C), and washing time (1–10 min). For all evaluated conditions, chromium removal was monitored by flame atomic absorption spectrometry. The residual tannery leather after different extraction strategies were characterized using a scanning electron microscopy. For the proposed method, the optimized conditions were: 3 g of residual tannery leather to be treated, 100 mL of extraction solution (chromium/complexant molar ratio of 1:3), at 80 °C and 30 min of sonication. To complete the chromium removal, only five washing cycles (50 mL of water at 50 °C) of 3 min were required. Using these conditions, a chromium removal higher than 98% was achieved. Under the same reaction conditions, the results were compared with mechanical stirring (100 rpm), which allowed observing the significant effects of ultrasound for chromium removal. Comparing to the conventional method, the total time of the process (including extraction and washing steps) was decreased from 150 to 45 min and the water volume for the washing was reduced from 450 to 250 mL. Therefore, the proposed ultrasound-assisted process can be considered as a suitable alternative for chromium removal from residual tannery leather.