In this work, we computationally explore two independent degrees of freedom in designing MFU-4ltype frameworks: the substitution of the central atom of the SBU and alteration of the peripheral binding atom. This is illustrated in Figure , which depicts a cluster model of the M I M II -MFU-4l SBU. Our objective is to understand how these two factors interplay and influence the overall performance of this class of materials. We will investigate various combinations of central and peripheral metal ions to identify parings that yield the most favorable binding enthalpies and usable capacities. By doing so, we computationally discover three combinations that not only meet but exceed the current material for hydrogen storage based on MFU-4l frameworks, paving the way for MFU-4-type materials that offer a balance of the high surface coverage at high pressure and the small surface coverage at the discharging pressures.