Aloe gel (Alg), which is a natural extract from the Aloe sp. plant, was evaluated in this study for its potential use as a bioflocculant to treat urban wastewater sewage sludge. The gel was used alone and combined with water glass (WG) under controlled conditions in laboratory experiments. Alg was found effective to settle the flocculated sludge rapidly and remove distinctive unpleasant odours of the sludge as highlighted by gas chromatography-mass spectrometry (GC/MS) analysis. Furthermore, Alg was pH tolerant and had no effect in changing the pH of the wastewater. The optimum dose of Alg was 3% at which a sludge volume index (SVI) of 45.4 mL/g was obtained within 30 min settling time. To enhance the treatment performances of Alg, WG was also evaluated as an alkali agent to further reduce the chemical oxygen demand (COD) and ammonia (NH4-N) in the wastewater. At equal doses of 3% of WG and Alg each, the combined treatment outcomes showed high turbidity and NH4-N removals of 83 and 89%, respectively, but the overall COD removal was at best 25%. The settling rate of treated sludge with combined Alg/WG was very rapid giving an SVI of 25.4 mL/g within only 5 min.