Membrane technology plays important roles in drinking water treatment in last decades; ultrafiltration (UF) is typically used to separate natural organic matters (NOM) and nanofiltration (NF) is used primarily to reject divalent ions, due to the different pore sizes of the used membranes. However, high water production rate at low energy consumption will be achieved if NOM and heavy metals can be simultaneously removed via UF-based water treatment process, which is necessary nowadays due to the carbon neutrality target worldwide. Here, a polyethersulfone (PES)-based UF membrane, modified chemically by grafting and crosslinking polyethylenimine (PEI, 25,000 Da) in two steps, was used to simultaneously remove humic acid (HA) and copper (Cu) from water. The molecular weight cut-off of the PEI-modified membrane was ∼110 kDa, and results showed that the efficiencies of HA and Cu2+ removal substantially increased because of the smaller pore size and additional adsorption effects compared to pristine PES membrane. Although the flux of the PEI-modified membrane was reduced, the membrane fouling was significantly alleviated compared with the pristine UF membrane. In comparison with Fe-based coagulants, Al-based coagulants as pretreatment performed better on removing HA and Cu2+, and the membrane flux greatly improved compared to only UF. The higher the coagulant dosage, the better the membrane performance was, particularly the pollutants removal efficiency. In addition, the PEI-modified UF membranes presented excellent pollutants removal after 4 months of storage in water. Besides, the as-modified UF membrane has only limited influence on removing mineral substances (e.g., Ca2+, Mg2+), indicating a potential application in actual water treatment. Furthermore, the PEI-modified membrane can be easily chemically cleaned; the removal efficiencies for hybrid Al-coagulation and UF process were as high as 88.2% ± 0.8% (HA) and 82.8% ± 0.1% (Cu2+) even after 4 cycles of filtration and subsequent chemical cleaning.