Ammonium persulfate modified mixed metal oxide derived from hydrotalcite with tunable acid/base properties can be prepared via thermal decomposition of Mg-Al hydrotalcite-type precursors and ammonium persulfate. By controlling the ammonium persulfate content, these sulphur mutated samples, denoted as SMgAlO-y (y = 1; 3; 5; 7), were investigated in this research. The resulted materials were characterized by XRD, SEM, FT-IR spectra, Py-IR spectra, XPS, Hammett indicator, CO2-TPD, as well as NH3-TPD. Furthermore, the acid-base property of the sample surface was determined by inverse gas chromatography measurements (IGC). Among all the obtained outcomes, the target SMgAlO-5 demonstrated the maximal Ka/Kb value, and it presented the highest activity as a catalyst in the synthesis of propylene carbonate (PC) through 1,2-propylene glycol and urea, giving the yield of 97.2% at the optimized reaction condition, which indicated that the PC yield counted on the synergic effect of the acidity and basicity on catalysts.