The removal efficiency of several pharmaceutically active compounds from two different surface water types was investigated. Two different nanofiltration (NF) membranes (Trisep TS-80 and Desal HL) were first studied at low feed water recoveries (10%). In a second phase, the combination of an NF unit at higher feed water recovery (80%) with subsequent granular activated carbon (GAC) filtration of the permeate was investigated. Results indicate that removal of the selected pharmaceuticals with NF is mainly influenced by charge effects: negatively charged solutes are better removed, compared with uncharged solutes, which are, in turn, better removed compared with positively charged solutes. This latter trend is mainly due to charge attractions between the negatively charged membrane surface and positively charged solutes. Increasing feed concentrations of positively charged pharmaceuticals lead to increasing rejection values, due to membrane charge-shielding effects. The removal efficiency of pharmaceuticals with the combination NF/GAC is extremely high. This is mainly due to an increased adsorption capacity of the activated carbon since the largest part of the natural organic matter (NOM) is removed in the NF step. This NOM normally competes with pharmaceuticals for adsorption sites on the carbon.