The anisotropic growth and the different interface properties of ionic crystal at microscale make it difficult to control and obtain the ordered crystals at macroscale, resulting in rare researches on self-assembly of ionic crystal. The method of evaporation-induced crystal self-assembly (EICSA) has been demonstrated for the construction of highly ordered self-assembly configurations in the sodium chloride (NaCl) drops regulated by trace of water-soluble organic polymer (polyacrylamide, PAM) on the hydrophobic substrate. According to the dynamic behaviors of self-assembly configurations, the concentration phase diagram of configurations is given, showing that EICSA is a process from disorder to order with the increase of the amount of PAM. We interpret this phenomenon as a result of the addition of PAM promotes the nucleation and inhibits the growth, producing a large number of NaCl with small size. Meanwhile, the adhesion of PAM makes NaCl orderly assembled together. Particularly, the mechanisms of the spontaneous lifting of crystals are directly revealed through our experiments. Moreover, we develop the lattice model to explain the physical mechanisms behind the evolution of self-assembly configurations. Furthermore, the dependence of the evaporating rate from regions (III) to (I) on the mixing free energy change is found to be consistent with the Arrhenius behavior. Our results have shown a further understanding of construction and control in self-assembly of ionic crystal, which has great applications in protection of outdoor electronics, conservation of cultural relics and chemical production.