Compressed sensing (CS) has been proposed to improve the efficiency of signal processing by simultaneously sampling and compressing the signal of interest under the assumption that the signal is sparse in a certain domain. This paper aims to improve the CS system performance by constructing a novel sparsifying dictionary and optimizing the measurement matrix. Owing to the adaptability and robustness of the Takenaka–Malmquist (TM) functions in system identification, the use of it as the basis function of a sparsifying dictionary makes the represented signal exhibit a sparser structure than the existing sparsifying dictionaries. To reduce the mutual coherence between the dictionary and the measurement matrix, an equiangular tight frame (ETF) based iterative minimization algorithm is proposed. In our approach, we modify the singular values without changing the properties of the corresponding Gram matrix of the sensing matrix to enhance the independence between the column vectors of the Gram matrix. Simulation results demonstrate the promising performance of the proposed algorithm as well as the superiority of the CS system, designed with the constructed sparsifying dictionary and the optimized measurement matrix, over existing ones in terms of signal recovery accuracy.