Crystalline 4-N, N-dimethylamino-4ʹ-Nʹ-methyl-stilbazolium tosylate (DAST) is known as an excellent organic nonlinear optical (NLO) material. However, it is vulnerable to damage caused by high-intensity laser irradiation, which severely limits its NLO applications. In this study, DAST molecules were included with β-cyclodextrin (β-CD), and DAST@β-CD supramolecular nanowires (NWs), microplates (MPs), and chaotic microcrystals (CMCs) were successfully prepared. All the crystals not only possess excellent NLO properties, but also exhibit greatly enhanced optical damage tolerances (ODTs) and photoluminescence. Under the pumping of a 532-nm picosecond (ps) pulsed laser, we achieved single-mode lasing from MPs and random lasing from CMCs, with thresholds of 55.22 and 88.38 nJ/cm2, respectively. When the laser irradiation had a peak intensity of ~17.5 GW/cm2, which is 8-9 orders of magnitude higher than the DAST bulk-crystal photobleaching intensity, the CMC laser emission intensity retained ~95% of its initial value after 4 h of operation in an ambient atmosphere.