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Surface modifications have great potential to control semiconductor properties such as band bending (BB) and electron affinity (EA). It is demonstrated that tailor-made, surface-binding molecules—discarboxylic acid derivatives with aromatic substituents in this case—can be used to modify systematically both the EA and BB of CdSe. The molecular parameters that affect each of these have been resolved and a semiquantitative model is put forward to rationalize the observed molecule-induced band-bending energies.