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ZnSe films have been grown on 〈100〉, 〈110〉, and 〈111〉B GaAs surfaces, using the metalorganic chemical vapor deposition technique. The electrical transport properties and lattice structure characteristics of these films have been studied using a van der Pauw technique and high‐resolution transmission electron microscopy. The electrical and structural properties of these films vary significantly with growth direction. In (100) layers, the observed defects are similar in nature to isolated compensated centers. For other orientations, observed properties are best described in terms of extended defects and grain boundaries.