X-ray diffraction, elemental analysis, scanning electron microscopy, and 2 9 Si magic angle spinning (MAS), 1 H- 1 3 C cross-polarization (CP) MAS and 1 H- 2 9 Si CP MAS NMR spectroscopies are used to study SSZ-24 synthesis from aqueous silicate mixtures containing alkali and N,N,N-trimethyl-l-adamantammonium (TMAA + ) cations. SSZ-24 only forms from mixtures prepared using fumed silica, KOH, and TMAAOH, with TMAA/Si≥0.15. SSZ-24 nuclei form through Van der Waals and coulombic interactions between the anionic silicate species and the TMAA + cations in the gelatinous synthesis mixture. The results cannot distinguish whether SSZ-24 nuclei form in the liquid or solid phase of the synthesis mixture. No evidence was found for occlusion of the TMAA + cations in the solid phase of the gel prior to SSZ-24 crystallization, suggesting that the rates of zeolite nucleation and crystallization may be comparable. Computer simulations reveal that the non-bonded interactions between TMAA + and the SSZ-24 lattice are weaker than the non-bonded interactions between tetrapropylammonium (TPA + ) cations and the silicalite-1 framework, which may explain why silicalite forms much faster than SSZ-24 when TPAOH is substituted for TMAAOH in the synthesis mixture.