The preparation of transdermal gels contained l-theanine was investigated as a preclinical study. The skin permeability of semisolid formulations of hydrophobic ointments, hydrophilic ointments, oily creams, creams, and lyogel containing theanine was compared and found that lyogel was the best. The composition of lyogel was also studied to obtain a formulation with good application comfort. Although it is suggested that this lyogel could be tested in clinical studies to determine whether it is effective for relief of PMS symptoms, lyogel may be suitable as an easy-to-use l-theanine-containing formulation for women that can relieve PMS symptoms.