A new mesoporous metal–organic framework (MOF; DUT‐60) was conceptually designed in silico using Zn4O6+ nodes, ditopic and tritopic linkers to explore the stability limits of framework architectures with ultrahigh porosity. The robust ith‐d topology of DUT‐60 provides an average bulk and shear modulus (4.97 GPa and 0.50 GPa, respectively) for this ultra‐porous framework, a key prerequisite to suppress pore collapse during desolvation. Subsequently, a cluster precursor approach, resulting in minimal side product formation in the solvothermal synthesis, was used to produce DUT‐60, a new crystalline framework with the highest recorded accessible pore volume (5.02 cm3 g−1) surpassing all known crystalline framework materials.