Recently, we have performed high-throughput simulations to quantify phase competition in zeolites. The large number of simulated zeolite-OSDA pairs allowed rationalizing historical synthesis outcomes from the literature, explaining accessibility windows, and aluminum distributions in single zeolite frameworks as a function of OSDA shape and charge distribution. Furthermore, the data was used to control the synthesis of an aluminosilicate CHA/AEI intergrowth with an OSDA with dual selectivity. By designing OSDAs with shapes and binding energies competitive towards the two frameworks forming the intergrowth, we have demonstrated that this disordered structure can be crystallized in its high-silica form. In this work, we extend these design principles towards several other intergrown zeolites by combining simulations and data mining. Starting from a dataset of hundreds of thousands of zeolite-OSDA pairs, we singled out potential bi-selective OSDAs for the synthesis of both known and hypothesized intergrowths. To demonstrate the applicability of the method towards small, medium, and large-pore zeolites, we designed potential bi-selective OSDAs for the CHA/AFX, MTT/TON, and BEC/ISV intergrowths. Finally, the strategy is extended to several known frameworks, and one example of a hypothesized intergrowth. This work is expected to accelerate the discovery of intergrowth zeolites through theory and simulations. This new computational strategy for designing an intergrowth zeolite is shown in Fig. . OSDAs known to be selective towards pure phase zeolites are used as references for the shape, such as N-ethyl-N-methyl-2,2,6,6-tetramethylpiperidinium for AEI and N,N,Ntrimethyladamantammonium for CHA (Fig. ). Then, new OSDAs for the intergrowth can be designed using phase competition and shape metrics. Binding metrics built upon binding energies were calculated for OSDAs retrieved from the literature and for chemically modified ones. 10, In particular, we define the competition energy by comparing the binding energies of one OSDA towards all calculated frameworks, and adopting the second-best zeolite-OSDA pair as the energy reference. This quantifies how strong are the phase competition effects for a given OSDA, with more negative values indicating less competition. Moreover, the shape of an OSDA is quantified by first projecting nuclear coordinates of the molecule into a two-dimensional space using a principal component analysis, and later measuring the two axes describing the molecule (see Supporting Information). 10 When designing bi-selective OSDAs for intergrowth systems, we postulate that an ideal bi-selective OSDA should: (i) be an equally strong binder towards both phases forming the intergrowth, (ii) be a weak binder towards all other competing phases (Fig. ), and (iii) have a geometry that is in-between the reference OSDAs in the shape space, thus favoring the crystallization of both structures (Fig. ). Beyond the previously demonstrated CHA/AEI intergrowth, we discuss the application of this method to many other intergrown zeolites of practical interest. For example, the highsilica CHA/AFX zeolite is used in applications such as MTO reaction, or selective catalytic reduction of NO x (NO x -SCR), but is typically synthesized using a mixture of OSDAs. Although both zeolites are ABC-6 structures and have cages with similar diameters, the aft cage in AFX zeolite is 40% longer than the cha cage. This discrepancy in size has led AFX to be synthesized with longer OSDAs, including diquaternary ammonium molecules such Along with the binding energies, bi-selective OSDAs should also satisfy c, shape matching requirements. Often, binding energy metrics give rise to selectivity domains in the shape space.