Owing to excellent mechanical properties, Al alloys are widely used in aerospace, automotive and civil industry. In order to optimize the properties and performance of the currently used Al alloys and/or even design novel Al alloys, the quantitative description of the microstructure during alloys preparation is the key. In recent years, the phase-field simulation coupling with the CALPHAD thermodynamic and atomic mobility databases has become an effective way to quantitatively simulate the microstructure evolution. So far, the accurate thermodynamic database for Al alloys has been established. However, it is not the case for atomic mobility database for Al alloys. The major obstacle lies in the lack of reliable diffusion coefficients in ternary and higher-order Al alloys, and thus there is an urgent need to remedy this situation. In this work, several semi-infinite and finite (thin film) single-phase solid-state diffusion couples in bcc Al-Fe-Mn and fcc Al-Cu-Ni alloys were first prepared. The concentration profiles for all the diffusion couples were then measured by means of EPMA. After that, the pragmatic numerical inverse method, which has been recently developed for high-throughput determination of the interdiffusion coeffi cients in ternary system and validated in several systems, was employed to compute the composition-dependent interdiffusivities in the corresponding systems at 1273 K. In order to eliminate the possibility that different interdiffusivities at the same composition would be obtained from different sets of diffusion couples, only one set of adjustable parameters was used for one system. All the obtained interdiffusivities satisfy the thermodynamic constrains. On the basis of the determined interdiffusivities as well as Fick's second law, all the experimental concentration profiles were reproduced nicely via numerical simulation, which verifies the reliability of the determined interdiffusivities. The further analysis indicates that the pragmatic numerical inverse method can not only realize the determination of reliable composition-dependent interdiffusion coefficients in ternary diffusion couples, but also cover the cases which cannot be dealt with by the traditional Matano-Kirkaldy method, such as the diffusion couples without intersection along their diffusion paths, and the finite (thin film) diffusion couples. In addition, the comparison between the interdiffusivities from semi-infinite diffusion couples and those from finite (thin film) diffusion couples was made, and the probable reason for their difference was also pointed out. All the presently obtained interdiffusivities in bcc Al-Fe-Mn and fcc Al-Cu-Ni alloys will be utilized to develop the accurate atomic mobility databases in ternary Al-Fe-Mn and Al-Cu-Ni systems in the next step.