A process for making a microlens array or a microlens array masterform comprises (a) providing a photoreactive composition, the photoreactive composition comprising (1) at least one reactive species that is capable of undergoing an acid- or radical-initiated chemical reaction, and (2) at least one multiphoton photoinitiator system; and (b) imagewise exposing at least a portion of the composition to light sufficient to cause simultaneous absorption of at least two photons, thereby inducing at least one acid- or radical-initiated chemical reaction where the composition is exposed to the light, the imagewise exposing being carried out in a pattern that is effective to define at least the surface of a plurality of microlenses, each of the microlenses having a principal axis and a focal length, and at least one of the microlenses being an aspherical microlens.