Zeolite synthesis results for the use of a family of related quaternary ammonium derivatives of tricyclodecane hydrocarbons as structure-directing agents are described. The work continues our interest in how rigid polycyclic hydrocarbons, as charged derivatives, occupy space in developing guest/host zeolite lattices. The zeolite product chemistry was probed as to the three-dimensional structures formed, particularly in relation to synthesis variables like boron substitution for silicon in the lattice, OH-/SiO2 reactant concentration, and the stereochemistry of the polar substituents off the tricyclo[5.2.1.0(2,6)]decane hydrocarbon frame; all three factors were found to have an impact on the zeolites which crystallized. Some correlations were also studied for how these factors influenced the size and architecture of the resulting pore systems. Monte Carlo methods were also applied to calculate favorable docking energies for geometry-optimized organo-cations placed in the host lattices.