The study of viscoelastic fluids as artificial tears dates back to the late 1970s. Healon, the first ophthalmic viscosurgical device, was approved in 1980, but studied extensively before then, exhibits very interesting shear-thinning properties that were found to be beneficial in both ophthalmic surgery and somewhat later as a tear replacement solution. Unlike the previous tear film replacements, which were mainly viscous in nature, viscoelastic solutions, particularly those based on hyaluronan, exhibited very interesting, potentially beneficial, rheological properties, especially when slightly altered to become elastoviscous. This review examines the rheological properties that are significant in artificial tear solutions. We define herein the necessary parameters that need to be further studied to design and formulate rheologically better artificial tears, which should provide enhanced efficacy compared with their predecessors.