In this work, an optimization-based inverse design method is provided for multi-input multi-output (MIMO) metastructured devices. Typically, optimization-based methods use a full-wave solver in conjunction with an optimization routine to design devices. Due to the computational cost this approach is not practical for designing electrically-large aperiodic metastructured devices. To address this issue, a 2-D circuit network solver using reduced order models of the metastructure's unit cells is introduced. The circuit network solver is used in conjunction with a gradient-based optimization routine that uses the adjoint variable method to solve large-scale optimization problems like those posed by metastructured devices. To validate the inverse design method, a planar beamformer and an analog signal processor for aperture field reconstruction are designed and validated with full-wave simulations.