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Dense linear layers are the dominant computational bottleneck in large neural networks, presenting a critical need for more efficient alternatives. Previous efforts focused on a small number of hand-crafted structured matrices and neglected to investigate whether these structures can surpass dense layers in terms of compute-optimal scaling laws when both the model size and training examples are optimally allocated. In this work, we present a unifying framework that enables searching among all linear operators expressible via an Einstein summation. This framework encompasses many previously proposed structures, such as low-rank, Kronecker, Tensor-Train, Block Tensor-Train (BTT), and Monarch, along with many novel structures. To analyze the framework, we develop a taxonomy of all such operators based on their computational and algebraic properties and show that differences in the compute-optimal scaling laws are mostly governed by a small number of variables that we introduce. Namely, a small ω (which measures parameter sharing) and large ψ (which measures the rank) reliably led to better scaling laws. Guided by the insight that full-rank structures that maximize parameters per unit of compute perform the best, we propose BTT-MoE, a novel Mixture-of-Experts (MoE) architecture obtained by sparsifying computation in the BTT structure. In contrast to the standard sparse MoE for each entire feed-forward network, BTT-MoE learns an MoE in every single linear layer of the model, including the projection matrices in the attention blocks. We find BTT-MoE provides a substantial compute-efficiency gain over dense layers and standard MoE.