Dissolved aluminum (Al) is a sensitive tracer for biogeochemical cycles in the ocean. There has been a dramatic decline in water and sediment fluxes into the sea from the Huanghe because of climate change and human activities. Water–Sediment Regulation Schemes (WSRSs) have been implemented annually to flush trapped sediments from the upstream watercourse and reservoirs of the river. Monthly observations to investigate the behavior of dissolved Al in the lower reach of the Huanghe were carried out from November 2008 to December 2010. During 2009, daily observations were made to assess the impact of the ninth WSRS on the lower reach of the Huanghe and three cruises were carried out in the Huanghe Estuary in 2009 (prior to, during and following the WSRS). The monthly concentrations of dissolved Al ranged from 25 nM to 362 nM (average 90 nM) in the lower reach of the Huanghe. Assessment of the seasonal variation of dissolved Al showed that the highest concentrations occurred in summer and the lowest in winter: these corresponded to the variations in water discharge and sediment loads, which were controlled by WSRS events. During the ninth WSRS events in 2009 the daily runoff and sediment load increased from 200 m3/s to 3600 m3/s and from 0.1 g/L to 5 g/L, respectively. The concentration of dissolved Al increased from 180 nM to 600 nM (average 380 nM) in less than 20 days, which were equivalent to 43% of the annual Al flux into the Bohai. Exchange between dissolved and particulate Al, investigated using a simple sorption model based on the distribution coefficient (Kd), was approximately 106 mL/g in the Huanghe. The average concentrations of dissolved Al in the Huanghe Estuary prior to, during and following the WSRS were 243 nM, 238 nM and 186 nM, respectively. The comparable concentrations of dissolved Al in the Huanghe Estuary prior to and during the WSRS indicate that removal processes occurred in the initial stages of mixing in the estuary. The Al–salinity relationship and laboratory mixing experiments demonstrated that dissolved Al has a non-conservative behavior in the Huanghe Estuary, where a significant loss (20–50%) occurred. The mechanism of removal of dissolved Al in the Huanghe Estuary was adsorption onto suspended particulate matter and salt-induced flocculation. These observations suggest that human activities (e.g. the WSRSs) and sorption processes dominate the geochemical interactions of Al in the Huanghe and its estuary.