Abstract: We demonstrate herein that weak CH...O hydrogen bonds (HB) play a significant role in zeolite structure direction using organocations. This type of HB were identified between alkyl groups of the organic structure directing agent (OSDA) and the silica framework in as synthesized silicalite-1 of complex topology (MFI) using a combination of experimental and theoretical data obtained at low and room temperatures. The 28 weak CH...O HB, evidenced along dynamics simulation at room

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... re, represent 30% of the energy of the Coulomb electrostatic interaction between OSDA and the zeolite framework. The strongest and most stable HB found here connects the OSDA to the [415262] cage containing F atoms and should contribute to preserve zeolite topology during crystal growth. An inspection of other as-synthesized zeolites of very different framework topology indicates that the directional CH...O HBs have to be considered when discussing zeolite structure directing phenomena.