Excimer laser processing enables both thermally-driven transformations and the incorporation of solutes into the surface of materials through melting and diffusional mixing. We have examined the effect of excimer laser processing on the microstructure and surface mechanical properties of titanium alloys. Changes in the surface hardness due to laser processing were studied using a Nanoindenter™. Alloying experiments using both mixing of evaporated surface layers of boron and laser gas alloying in air and in nitrogen all result in changes in the surface hardness of the material. Alloying with boron results in an amorphous surface which is somewhat harder than the as polished surface. Laser processing in air and pure nitrogen results in incorporation of oxygen and nitrogen and the development of fine precipitates of TiO and TiN respectively. Substantial increases in surface hardness result due to solution and precipitation mechanisms. Nanoindenter™ data from several depths in the material are correlated with microstructure and solute concentration to illuminate the strengthening mechanisms involved.