Amorphic diamond films can be prepared at room temperature with a laser plasma discharge source of multiply charged carbon ions without the use of any catalyst. Composed of packed nanophase nodules, in which the carbon atoms are linked with the tetrahedral bonding of diamond, these noncrystalline films adhere readily to most every material that is used in current industrial applications. The high energy of condensation causes deep penetration of carbon atoms into the substrates, where they form significant interfacial layers. In this work, the adhesion properties of amorphic diamond films deposited on zinc sulfide substrates were studied. It was shown that the adhesion of the films was inversely correlated with the amount of zinc hydride impurity in the substrate. In addition, the role of Zn-C additives to the natural interlayer between films and zinc sulfide substrates was investigated. The interface was built layer by layer by alternating the laser focus between feedstocks of zinc sulfide and graphite according to a program. The adhesion properties of the resulting structures are given.