A method of forming an organic solid crystal (OSC) thin film includes forming a layer of a non-volatile medium material over a surface of a mold, forming a layer of a molecular feedstock over a surface of the non-volatile medium material, the molecular feedstock including an organic solid crystal precursor, forming crystal nuclei from the organic solid crystal precursor, and growing the crystal nuclei to form the organic solid crystal thin film. An organic solid crystal (OSC) thin film may include a biaxially-oriented organic solid crystal layer having mutually orthogonal refractive indices, n1≠n2≠n3.