Phosphate, which contains the essential element phosphorous (P), is a necessary fertilizer for agriculture, but the current phosphate deposits are running out and alternative sources are needed. Sludge obtained from wastewater treatment plants contains high concentrations of phosphorus and represents an alternative, sustainable source. In this study, sludge obtained from a wastewater treatment plant with biological and chemical phosphorus removal was acidified (pH = 3, 4, 5 and 6) to release orthophosphate followed by sequestration of the orthophosphate by a zinc aluminum layered double hydroxide (Zn2Al-LDH). Sulfuric acid (H2SO4), nitric acid (HNO3), and hydrochloric acid (HCl) was tested, which showed that only sulfate anions compete with phosphate and results in reduced phosphate recovery (25-35%). The orthophosphate concentration in the liquid phase increased from 20% (raw sludge) to 75% of the total phosphorus concentration at a pH of 3, which enhanced the phosphate uptake by the ZnAl-LDH from 1.7 ± 0.2% to 60.3 ± 0.6%. During acidification, the competing anion carbonate is degassed as CO2, which further improved the phosphate uptake. PXRD showed the intercalation of carbonate in the LDH in the raw sludge at pH = 8, whereas orthophosphate was intercalated at lower pH values. 27Al MAS NMR spectroscopy and powder X-ray diffraction (PXRD) proved preservation of the LDH at all pH values. Furthermore, about a fourth of the Al is present as an amorphous aluminum phosphate (AlPO4) upon exposure to phosphate at low pH (pH = 3 and 5) based on 27Al MAS NMR spectroscopy. At a pH of 6 about a third of the P is present as brushite (CaHPO4·2H2O).