A Vertical Cavity Surface Emitting Laser (VCSEL) assembly including a VCSEL structure having a light-emitting region located on its surface, a relatively wettable region of a surface modifier coating formed over the light emitting region, and a microlens formed on the relatively wettable region. A relatively non-wettable region of the surface modifier coating is formed around the light-emitting region (e.g., on the electrode surrounding the light-emitting region). The surface modifier coating is formed, for example, from one or more organothiols that change the surface energies of the light-emitting region and/or the electrode to facilitate self-assembly and self-registration of the microlens material. The microlens material is printed, microjetted, or dip coated onto the VCSEL structure such that the microlens material wets to the relatively wettable region, thereby forming a liquid bead that is reliably positioned over the light-emitting region. The liquid bead is then cured to form the microlens.