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Recently, tensor decompositions continue to emerge and receive increasing attention. Selecting a suitable tensor decomposition to exactly capture the low-rank structures behind the data is at the heart of the tensor decomposition field, which remains a challenging and relatively under-explored problem. Current tensor decomposition structure search methods are still confined by a fixed factor-interaction family (e.g., tensor contraction) and cannot deliver the mixture of decompositions. To address this problem, we elaborately design a mixture-of-experts-based tensor decomposition structure search framework (termed as TenExp), which allows us to dynamically select and activate suitable tensor decompositions in an unsupervised fashion. This framework enjoys two unique advantages over the state-of-the-art tensor decomposition structure search methods. Firstly, TenExp can provide a suitable single decomposition beyond a fixed factor-interaction family. Secondly, TenExp can deliver a suitable mixture of decompositions beyond a single decomposition. Theoretically, we also provide the approximation error bound of TenExp, which reveals the approximation capability of TenExp. Extensive experiments on both synthetic and realistic datasets demonstrate the superiority of the proposed TenExp compared to the state-of-the-art tensor decomposition-based methods.