This study investigates an innovative dechlorination process using anaerobic granular sludge that was partially exposed to oxygen. The exposure supported a synchronously anaerobic and aerobic bioconversion process that combined reductive dechlorination with aerobic co-oxidation in a sludge granule. Experimental results showed that the highest dechlorination rates of tetrachloroethene, trichloroethene, cis-dichloroethene and vinyl chloride were 6.44, 2.98, 1.70 and 0.97 nmol/gVS day, at initial O2 concentrations of 10, 100, 5 and 0%, respectively. Strictly anaerobic conditions favored the dechlorination of vinyl chloride while absolutely aerobic conditions were preferred for trichloroethene dechlorination. Microaerophilic conditions are suggested to ensure the overall biodegradation of the chlorinated ethenes present in groundwater as a mixture.