We discover that the crystal morphology of zeolite-LTL could be modified by crown ether (21-crown-7, CE), where CE decreases the aspect ratio of zeolite-LTL while increasing the nucleation of domains on the (0001) face and hindering their growth along the c-axes. Moreover, the study using scanning electron microscopy supports that the ratio between the rates for generation of cancrinite columns and bridging cancrinite columns on the {10 (1) over bar0} face remains constant among the LTL frameworks with different amounts of CE molecules. In addition, X-ray diffraction analysis shows that potassium cations redistribute into pore cavities (t-lil) from cancrinite cages (t-can) and t-ste cages by the strong interactions between potassium and CE as the amount of CE molecules is increased. Additionally, Monte Carlo simulations clarify that stabilization of the t-lil cage via the redistribution of potassium cations at high CE concentration is attributed to the dominant effect in the crystal morphology changes observed. To understand the catalytic and adsorption properties of zeolites, it is important to investigate their structure/property relationships. Especially, studying the morphology of an anisotropic zeolite crystals has been of great interest because of the strong influence on controlling its properties. Thus, morphological control of the material with a particular crystallographic direction is highly desirable to obtain maximum properties for applications.