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We have examined the effect of composition on the Raman-active vibrational response of the Cu2(FexZn1−x)SnS4and Cu2(MnxZn1−x)SnS4solid solution series at ambient conditions. Based on these results we were able to identify the phase boundaries of the respective kesterite-type and stannite-type structures adopted by these compounds as a function of composition. In the case of Cu2(FexZn1−x)SnS4, our observations correlate very well with earlier reports. For the Cu2(MnxZn1−x)SnS4series, on the other hand, we were able to clearly pinpoint the kesterite↔stannite transition for intermediate compositions for the first time, indicating that Raman spectroscopy can serve as an efficient method for monitoring subtle structural transitions in these systems.