Metalorganic deposition (MOD) is a nonvacuum method of thin‐film deposition which allows easy alteration of chemical components and is compatible with thin‐film processing. We report the preparation of thin‐film superconductors by MOD. Rutherford backscattering spectrometry was used to determine film compositions and thicknesses. Films, approximately 500 nm thick, of YBa2Cu4Oz(zundetermined) were deposited on ⟨100⟩ single‐crystal SrTiO3. A superconducting onset temperature of 90 K was measured with 37 K the zero resistance temperature. Scanning electron microscopy revealed grain sizes approximately 250 nm in diameter.