CdTe nanocrystals were prepared in aqueous solution via the reaction between Cd2+ and NaHTe in the presence of mercaptoacetic acid. Interactions between CdTe nanocrystals and phenylalanine were formed via electrostatic/coordinate self-assembly. The photoluminescence intensity of CdTe nanocrystals was improved obviously. The interaction mechanism was discussed and was considered to be surface passivation.