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Estimation of covariance components in the multivariate random-effect model with nested covariance structure is discussed. There are two covariance matrices to be estimated, namely, the between-group and the within-group covariance matrices. These two covariance matrices are most often estimated by forming a multivariate analysis of variance and equating mean square matrices to their expectations. Such a procedure involves taking the difference between the between-group mean square and the within-group mean square matrices, and often produces an estimated between-group covariance matrix that is not nonnegative definite. We present estimators of the two covariance matrices that are always proper covariance matrices. The estimators are the restricted maximum likelihood estimators if the random effects are normally distributed. The estimation procedure is extended to more complicated models, including the twofold nested and the mixed-effect models. A numerical example is presented to illustrate the use of the estimation procedure.