We present composition-controlled synthesis of ZnO-Zn composite nanoparticles by laser ablation of a zinc metal target in pure water or in aqueous solution of sodium dodecyl sulfate (SDS). By SDS concentration, composition and size of the nanoparticles can be controlled in a wide range. Relative amounts of the components Zn and ZnO, the particle size, and the microstructure can evolve with SDS concentration in solution. High SDS concentration corresponds to high relative amount of Zn nanoparticles existing as the core in the core/ shell nanostructures, whereas low SDS concentration leads to high ZnO amount. This was explained by a dynamic mechanism on the basis of the competition between aqueous oxidation and SDS capping protection. Correspondingly, optical absorption spectra evolve from the excitonic peak of ZnO (about 350 nm) to the Zn surface plasmon resonance (about 242 nm) with rise of SDS concentration. A blue (about 450 nm) photoluminescence was observed in the obtained ZnO nanoparticles, which was attributed to existence of interstitial zinc in ZnO lattices. This study has revealed that laser ablation of active metal in liquid media is an appropriate method to synthesize a series of metal oxide semiconductor-metal composite nanoparticles with controlled composition and size.