This exploratory study compares one pristine NdGaO₃(110) crystal with one crystal irradiated at 1 × 10¹¹ ions cm⁻² and one crystal irradiated at 1 × 10¹² ions cm⁻² using 147 MeV ⁸⁴Kr ions. Because each condition is represented by a single independent specimen, specimen-to-specimen variability is confounded with the irradiation condition, and no specimen-level statistical inference is made. Symmetric X-ray diffraction, condition-averaged confocal micro-Raman spectroscopy, and UV–Vis–NIR transmission were used to compare surface-normal lattice response, local vibrational line shapes, and radiation-induced optical attenuation. The nearly angle-independent XRD shift at 1 × 10¹¹ ions cm⁻² is dominated by a common angular offset, whereas the two surviving harmonics at 1 × 10¹² ions cm⁻² give a model-conditioned estimate ε₁₁₀ = +0.509 ± 0.040%. At the higher fluence, the integrated intensities captured in the coupled θ–2θ condition decrease to 9.35 ± 0.46% for (110) and 1.29 ± 0.06% for (220), while the (220) FWHM ratio reaches 7.83 ± 0.73. These fit-derived errors do not include specimen alignment or between-specimen variability. The archived condition-averaged Raman spectra retain Pbnm-like vibrational groups, while the fitted FWHM values of the 168, 214/215, and 449–470 cm⁻¹ features increase by 15.7%, 19.4%, and 14.8%. The bulk-integrated Nd³⁺ 4f–4f maxima remain stable within the wavelength sampling, whereas the effective R_p-normalized differential attenuation at 275–285 nm reaches 388.7 cm⁻¹. The data support an exploratory description of a strained and diffraction-heterogeneous crystalline layer; complete amorphization, quantitative mosaicity, a damage threshold, track dimensions, and a microscopic defect identity are not established.