The nonlinear optical (NLO) properties of organic crystals are susceptible to their molecular structure and stability under extreme conditions. Herein, the (2E)-2-(3,4-dimethoxybenzylidene)-3,4-dihydronaphthalen-1(2H)-one (DMP) chalcone crystal was synthesized and grown by a slow evaporation method, and its structural and optical responses under acoustic shock wave exposures were systematically investigated. Although previous reports indicate that the present crystal is thermally stable only up to 187 °C, the present work demonstrated remarkable resilience by withstanding transient acoustic shock conditions of approximately 0.59 MPa and 520 K without any signs of structural degradation, thereby demonstrating impressive resilience. XRD analysis indicated that no new diffraction peaks appeared after the shock exposure, confirming excellent phase stability of the crystal, while the variation in diffraction intensities and crystallite size indicated dynamic recrystallization. The crystallite size increased from 19 nm to 25 nm, which is accompanied by a decrease in lattice strain, indicating improvement in crystallinity. Further, optical microscopy showed a sequential process of defect creation and healing, and the crystal surface smoothed after the fourth and fifth shocks, consistent with shock-induced recrystallization. UV-Vis spectroscopy revealed a significant increase in optical transmittance from 31.6% to 71.5% and a slight modulation of the optical band gap from 3.21 eV to 3.32 eV, reflecting improved molecular ordering and reduced defect density. Overall, the structure remains stable while the band gap is tuned under acoustic shock waves, demonstrating that optical properties can be effectively modulated without disrupting the crystalline framework. This highlights acoustic shock wave exposure as a promising route for developing robust optoelectronic materials capable of reliable performance under extreme conditions. The findings further suggest that the acoustic shock wave technique can be used to engineer the microstructure and optical response of organic NLO crystals such as DMP, thereby expanding their potential for high-performance photonic and optoelectronic applications.