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A recent analysis of the optimization of magnetization transfer experiments to estimate first-order rate constants is extended to the design of experiments for measuring these constants and T1 when both parameters are initially unknown. When the number of measurement times is fixed, an optimal design will consist of a set of measurement times which ensures that the precision of the estimates of the combination of k and T1 is as small as possible in a worst-case scenario. Simple expressions are given for the parameters that characterize the optimal design.