Molybdenum disulfide has recently raised more and more interest due to its layer-related properties and potential applications in optoelectronics and electronics. Here, layer-controlled large-area and continuous MoS2 atomic layers were obtained on mica substrate by thermally decomposing ammonium thiomolybdate. The obtained MoS2 film is three layers uniformly. Because of the small lattice mismatch between MoS2 and mica, the epitaxial MoS2 film is well grown on the substrate. The as-grown MoS2/mica substrate is demonstrated to be suitable as a substrate for enhancing Raman signals of adsorbed molecules without any modification, which even can compare with graphene and will expand the application of MoS2 to microanalysis. (C) 2015 Elsevier B.V. All rights reserved.