This article focuses on the intralayer-dependent impulsive synchronization of multiple mismatched multilayer neural networks (NNs) with mode-mixed effects. Initially, a novel multilayer NN model that removes the one-to-one interlayer coupling constraint and introduces nonidentical model parameters is first established to meet diverse modeling requirements in complex applications. To help the multilayer target NNs with mismatched connection coefficients and time delays achieve synchronization, the hybrid controller is designed using intralayer-dependent impulsive control and switched feedback control approaches. Furthermore, the mode-mixed effects caused by the intralayer coupling delays and switched intralayer topologies are incorporated into the novel model and analysis method to ensure that the subsystems operating within the current switching interval can effectively use the topology information of the previous switching intervals. Then, a novel analysis framework including super-Laplacian matrix, augmented matrix, and mode-mixed methods is developed to derive the synchronization results. Finally, the main results are verified via the numerical simulation with secure communication.